Air quality in the Mexico City Metropolitan Area (MCMA) is the subject of many studies due to concerns from high emissions and their adverse effects on public health and the environment. In this study, a high resolution simulation is performed with the Community Multi-scale Air Quality modeling system (CMAQ) using meteorology generated by the Weather Research Forecasting system (WRF). The boundary conditions for CMAQ are provided by the Goddard Earth Observing System-CHEMistry model (GEOS-Chem). The simulation period was March 2-7, 2006. Hourly species concentrations of O3, NOx, CO, SO2, PM10, and PM2.5 for the period were provided by the Automatic Air Quality Monitoring Network (labeled as RAMA). Preliminary evaluation showed GEOS-Chem and CMAQ being in good agreement with their predicted concentrations. In comparison with the base case boundary conditions, the GEOS-Chem case performs better and predicts closer to the observed values of O3, NOx, PM10, PM2.5, and SO2. Particle trajectory analysis was performed using the HYbrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) to ascertain the major sources of SO2 emitters and their impact on the MCMA.

Isoprene emissions affect human health, air quality, and the oxidative capacity of the atmosphere. Globally anthropogenic non-methane volatile organic compounds (NMVOC) emissions are lower than that of isoprene, but local hotspots are hazardous to human health and air quality. In Africa the tropics are a large source of isoprene, while Nigeria appears as a large contributor to regional anthropogenic NMVOC emissions. I make extensive use of space-based formaldehyde (HCHO) observations from the Ozone Monitoring Instrument (OMI) and the chemical transport model (CTM) GEOS-Chem to estimate and examine seasonality of isoprene emissions across Africa, and identify sources and air quality consequences of anthropogenic NMVOC emissions in Nigeria. / Earth and Planetary Sciences

Mineral dust aerosols, the tiny soil particles in the atmosphere, play a key role in the atmospheric radiation budget through their radiative and cloud condensation nuclei effects. It is therefore important to evaluate the radiative forcing of mineral dust and subsequent changes in atmospheric dynamics. The Weather Research and Forecasting with Chemistry (WRF/Chem) regional model with the integrated dust modules and available observations have been used to investigate the three-dimensional distribution of mineral dust over Australia. Additionally, the WRF/Chem model was used to estimate the direct radiative forcing by mineral dust over Australia. Particular emphasize has been given to direct radiative feedback effect of mineral dust on boundary layer dynamics. Two dust emission schemes embedded within the WRF/Chem model have been utilized in this study: the dust transport (DUSTRAN) and the Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) schemes. The refractive index of mineral dust depends on the mineralogy, size and composition of dust over a given region. The refractive index of mineral dust for shortwave radiation was considered to be wavelength independent and set based on previous mineralogical studies over North Africa and Australia. However, the refractive index of mineral dust for longwave radiation was considered to be wavelength dependent and to vary for 16 longwave spectral bands. Model results were compared with observations to validate the performance of the model, including satellite datasets from the Moderate Resolution Imaging Spectroradiometer (MODIS), Multi-angle Imaging SpectroRadiometer (MISR) and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), as well as ground-based measurements obtained from air quality monitoring sites over Australia. The major results can be summarized as follows: (1) Lake Eyre Basin is the most important source of dust in Australia, with a peak activity identified to be during austral spring and summer, and dust emission within the basin is often associated with the passage of dry cold fronts; (2) Mineral dust from Lake Eyre Basin can be transported long distances to southeastern Australia in association with eastward propagating frontal systems, reaching as far as New Zealand and beyond, and to northern tropical Australia by postfrontal southerly winds, and subsequently towards northwestern Australia and the Indian Ocean by southeasterly trade winds; (3) Australian dust plumes are mainly transported in the lower atmosphere, although variation of boundary layer depth during the passage of cold frontal systems, as well as ascending motion at the leading edge of these systems and descending motion where postfrontal anticyclonic circulation is dominant contribute to the vertical extent of mineral dust aerosols; (4) the shortwave direct radiative effect of mineral dust results in cooling of the atmosphere from the surface to near the boundary layer top, but warming of the boundary layer top and lower free atmosphere; (5) changes in the vertical profile of temperature result in an overall decrease of wind speed in the lower boundary layer and an increase within the upper boundary layer and lower free atmosphere; (6) the longwave warming effect of mineral dust partly offsets its shortwave cooling effect at the surface. This compensation is significantly larger over and immediately downwind of dust source regions where coarse particles are more abundant, as they have stronger interaction with longwave radiation emitted from the Earth’s surface; (7) both shortwave and longwave radiative forcing by mineral dust was found to have a diurnal variation in response to changes in solar zenith angle and in the intensity of longwave radiation, respectively; (8) the absorptive nature of dust was shown to be associated with the shortwave heating of the atmosphere; (9) on the other hand, longwave cooling of the atmosphere was identified because absorption of longwave radiation by dust is less than its emission to the surface and top of the atmosphere (TOA).

Air quality modeling is a recent development in atmospheric science dedicated to simulating the characteristics of surface emissions within the context of a variety of meteorological conditions. In western Kentucky, there are several concentrated animal feeding operations (CAFOs) that emit a variety of gases, including sulfur dioxide (SO2). The hypothesis was that the concentration and spread of SO2 emissions from these sources would differ between wet and dry periods over the CAFO locations. In this thesis, point emissions from locations representing CAFOs in western Kentucky and the transit of SO2throughout the southeastern U.S. were simulated in multiple sensitivity experiments using the Weather Research and Forecasting model with Chemistry (WRFChem). Simulations were performed for the convective precipitation events that occurred over western Kentucky between July 7 and July 13, 2012. The spatial coverage of SO2 emissions originating from the locations was reduced during precipitation events and expanded during dry periods. The average concentration of SO2 over the study area was also higher during the breaks between precipitation events than during times when precipitation was occurring. The highest concentrations of SO2 exceeding 1,000 pptv remained within close range of the emission locations for the majority of the simulations, except for when local surface winds were blowing at higher speeds. Most emissions from the locations remained limited to the surface and 850 mb levels.

O objetivo deste trabalho foi o analisar o impacto da resolução dos conjuntos de dados topográficos nas simulações das concentrações de dióxido de enxofre (SO2) emitido por uma fonte localizada no Sul do Brasil. Para isso foram realizadas duas simulações aplicando o modelo regional Weather Research and Forecasting acoplado com a química (WRF/Chem), configurado com duas representações do terreno de diferentes resoluções espaciais. Foram utilizados os dados padrão do modelo com melhor resolução, Global 30 Arc-Second Elevation (GTOPO), com aproximadamente 1 km, e inserido no bancos de dados do modelo as informações de terreno em alta-resolução do Radar Shuttle Topography Mission (SRTM) (30 metros). Para as emissões antrópicas do modelo foi elaborado um programa capaz inserir os volumes do poluente SO2 de forma horária expelidos pela chaminé, de acordo com as taxas de emissão medidos diretamente na fonte. O programa representou a emissão do poluente no ponto de grade correspondente a localização e a altura acima da superfície da chaminé da fonte. As simulações foram configuradas com os seguintes esquemas de parametrização: para microfísica de nuvens foi utilizado o Goddard Cumulus Ensemble; os esquemas de radiação de onda longa e curta foram o Goddard e o Rapid Radiative Transfer Model para modelos de circulação geral da atmosfera (MCGA); para a parametrização de cumulus o esquema utilizado foi o Grell 3D Ensemble Scheme; e para os esquemas de camada superficial e camada limite planetária foram utilizados os da teoria da similaridade do Fifth-Generation National Center for Atmospheric Research/Penn State Mesoscale Model (MM5) e o Yonsey University, respectivamente. A escolha desta combinação de esquemas foi definida a partir de um estudo inicial da sensibilidade do modelo à mudança das parametrizações. Os resultados dos experimentos numéricos alterando a topografia foram validados a partir dos dados de monitoramento das estações meteorológica e da qualidade do ar pertencentes à empresa responsável pelo empreendimento associado à fonte. Foi observado que as simulações com os dados SRTM expressaram o terreno da região de estudo mais próximo à realidade, representando o aspecto heterogêneo do relevo, ressaltando os picos e os vales. Os resultados das validações meteorológicas utilizando os dados topográficos indicaram melhoras nas simulações das variáveis meteorológicas: temperatura, umidade relativa, velocidade do vento e precipitação. Os experimentos com os dados topográficos GTOPO e SRTM no modelo WRF/Chem, configurado com as emissões horárias da fonte de Candiota, reproduziram o comportamento dos ventos para transporte de SO2 até as estações de monitoramento conforme os dados observados. Porém foram identificados padrões diferentes na representação das concentrações do poluente entre as duas simulações do modelo, associados aos escoamentos dos ventos representados pelos experimentos. A resolução da topografia afetou na simulação de SO2 devido ao aumento da forçante superficial induzida pelo terreno. Este aumento na forçante, influenciou a advecção da pluma de SO2, resultando em diferentes padrões das concentrações de SO2 no ponto de grade correspondente às estações de monitoramento. Contudo, os resultados das simulações das concentrações de SO2, tanto de forma horária quanto na abordagem das médias diárias, não indicaram uma relação linear entre a utilização de dados em alta resolução e a melhora na representação do SO2 pelo modelo WRF/Chem. / The objective of this work was to analyze the impact of the higher resolution topographic data sets in the simulations of the Sulfur dioxide (SO2) concentrations emitted by a source located Southern Brazil. Two simulations were performed applying the Weather Research and Forecasting model coupled with Chemistry – WRF/Chem, configured with two representations of the terrain with different spatial resolutions. The standard data of the model with the best resolution (approximately 1 km), Global 30 Arc-Second Elevation (GTOPO), and was inserted in the model databases the high-resolution (30 meters) terrain information of the Radar Shuttle Topography Mission (SRTM). For the anthropic emissions of the model, a program was developed capable of inserting the hourly SO2 pollutant volumes expelled by the chimney, according to the emission rates measured directly at the source. The program inserted these emissions into the grid point corresponding to the location and height above the surface of the emission source. The simulations were configured with the following parameterization schemes: for cloud microphysics Goddard Cumulus Ensemble; for the long and short wave radiation treatment it was used the Goddard and the Rapid Radiative Transfer Model for general circulation models; for the cumulus parameterization the scheme it was used the Grell 3D Ensemble Scheme; and for the surface layer and planetary boundary layer schemes, the similarity theory of the Fifth-Generation National Center for Atmospheric Research/Penn State Mesoscale Model (MM5) and the Yonsey University, respectively. The choice of this combination of schemes was defined from an initial study of the sensitivity of the model to the change of parametrizations. The results of the numerical experiments altering the topography were validated from the monitoring data of the meteorological stations and the air quality belonging to the company responsible for the enterprise associated to the source. It was observed that the simulations with the SRTM data expressed the terrain of the region of study closest to reality, representing the heterogeneous aspect of the terrain, highlighting the peaks and valleys. The results of the meteorological validations using the new topographic data indicated an improvement in the simulations of the meteorological variables: temperature, relative humidity, wind speed and precipitation. The experiments with the GTOPO and SRTM topographic data in WRF/Chem model, configured with the hourly emissions of the Candiota source, reproduced the winds behavior that transported the SO2 to the monitoring stations according to the observed data. However, different patterns were identified in the pollutant concentrations between the two simulations of the model, associated to the wind flows represented by the experiments. The topography resolution affected in the simulation of SO2 due to the increase of the surface forcing induced by the terrain. This increase in the forcing influenced the advection of the SO2 plume, resulting in different patterns of SO2 concentrations at the grid point corresponding to the monitoring stations. However, the results of simulations of SO2 concentrations, both hourly and in the approach of daily averages, did not indicate a linear relationship between the use of high resolution data and the improvement in the representation of SO2 by WRF/Chem model.

Atmospheric trace components play a critical role in the earth–atmosphere system through their interaction and perturbation to global atmospheric chemistry. They perturb the climate through scattering and absorbing of solar radiation (direct effects), thereby impacting on the heat energy balance of the atmosphere, and alter cloud microphysical properties affecting cloud formation, cloud lifetime and precipitation formation (indirect effects). These trace components can also have adverse effects on human health, visibility and air quality (AQ) composition, including various feedback processes on the state of the atmosphere. As well as their direct and indirect effects, aerosols are important for cloud formation. They serve as cloud condensation and ice nuclei (CCN and IN) during cloud droplet and ice crystal formations. Although many connections between clouds and aerosol effects have been established in cloud physics and climate modelling, aerosol–cloud interaction (ACI) is still one of the areas of large uncertainties in modern climate and weather projections. Different models have been developed placing much emphasis on ACIs, to have robust and more consistent description processes within the meteorological and chemical variables to account for ACIs and feedback processes. Because pollutant distributions are controlled by a specific meteorology that promotes residence times and vertical mixing in the atmosphere, reliable chemical composition measurements are required to understand the changes occurring in the earth–atmosphere system. Also, because atmospheric pollution is a combination of both natural and man-made (anthropogenic) sources, to direct controlled and/or mitigation procedures efficiently, contributions of different sources need to be considered. Occasionally these are explored from a particular region or global environment, depending on a specific area of interest. A fully coupled online meteorology–chemistry model framework (WRF-Chem) is used to investigate atmospheric ACIs over southern Africa –a region characterized by a strong and intense seasonal biomass burning (BB) cycle. The large transport of aerosol plumes originating from the seasonal burning from agriculture, land-use management and various activities give rise to a unique situation warranting special scrutiny. Simulations are conducted for the 2008 dry season BB episode, implementing a chemical dataset from various emission sources (anthropogenic, BB, biogenic, dust and sea salt) with the meteorological conditions. A base line (CNTRL) simulation was conducted with all emission sources from 26 August to 10 September 2008. To probe the contribution of BB on the regional pollution and influence on ACIs, a sensitivity (TEST) simulation was conducted without BB emissions and compared to the base line. The impact of natural and anthropogenic aerosol particles is studied and quantified for the two simulations, focusing on aerosol concentration and cloud responses under different model resolutions. A statistical analysis of pollutant concentration of major regulated species and cloud variables is conducted and the percentage difference used to assess the contribution due to BB emissions. Results confirm the high variability of spatial and temporal patterns of chemical species, with the greatest discrepancies occurring in the tropical forests whereas the subtropics show more urban/industrial related emissions. Whilst CO and O3 show statistically significant increases over a number of cities/towns, the trend and spatial variability is much less uniform with NO2 and PM in most urban and populous cities. Statistical analysis of major chemical pollutants was mainly influenced by BB emissions. O3, NOx, CO and PM increase by 24%, 76%, 51%, 46% and 41% over the main source regions, whereas in the less affected regions concentrations increased by 5%, 5%, 5%, 3% and 2% when BB emissions are included. This study sheds new light on the response of cloud processes to changing aerosol concentrations and different model resolutions. In the parameterised case (dx = 20 km), clouds become more cellular, correlated with high supersaturations, whereas in the resolved case (dx = 4 km), they become more faint with relatively lower supersaturations. Aerosol effects on cloud properties were further studied and statistical analysis conducted on CCN, cloud droplet number concentration (CDNC), supersaturation and aerosol optical depth (AOD) at two different grid spacings. Most clouds occur to the west of the domain coincident with increase in aerosol concentration and AOD, while single scattering albedo (SSA) decreases. A considerable cloud ‘burn-off’ occurs in tropical west Africa, where aerosols can also be lofted up to 500-hPa level when BB emissions are included in the simulation. Due to BB, absorbing aerosol increased by 76% and 23% over tropical west and subtropical southeast, while tropical east shows no change. The study shows that tropical central Africa is characterized by an increased build-up in biomass burning aerosols (BBAs), forming a regional haze with high AOD; this becomes stronger near active burning areas with a significant proportion occurring to the west. AOD enhancement increases up to 38%, 31% and 11% in the west, east and south respectively. Although CDNC increased in areas with high aerosol concentration, supersaturation decreases (in the small domains) since increase in aerosol number concentration decreases maximum supersaturation Smax. Changes in absorbed radiation increased by +56 Wm-2, +23 Wm-2 and +14 Wm-2 in the west, east and southeast. To further evaluate the model sensitivity and its skill, an analysis was conducted by comparing the model performance with measurement data. Simulated AOD, surface concentrations of CO and O3, ozonesondes and liquid water path (LWP) were compared with measured data from MODIS satellite, SAFARI2000 field study and Cape Point WMO. The model shows a good skill in capturing and reproducing the trends as that measured. However, a severe lack of measurement data over southern Africa makes it more difficult to effectively evaluate WRF-Chem over southern Africa. There is a need for increased availability of measurements to adequately compare with models. This study is one of the first WRF-Chem studies conducted over southern Africa to simulate the weather and pollution interaction. The novelty of the present study is the combined analysis of ACI sensitivity to aerosol loading and cloud response in a regime-based approach. The study concludes with a brief discusssion of future directions for work on AQ and modelling interactions between pollution and weather over southern Africa.

O objetivo deste trabalho foi o analisar o impacto da resolução dos conjuntos de dados topográficos nas simulações das concentrações de dióxido de enxofre (SO2) emitido por uma fonte localizada no Sul do Brasil. Para isso foram realizadas duas simulações aplicando o modelo regional Weather Research and Forecasting acoplado com a química (WRF/Chem), configurado com duas representações do terreno de diferentes resoluções espaciais. Foram utilizados os dados padrão do modelo com melhor resolução, Global 30 Arc-Second Elevation (GTOPO), com aproximadamente 1 km, e inserido no bancos de dados do modelo as informações de terreno em alta-resolução do Radar Shuttle Topography Mission (SRTM) (30 metros). Para as emissões antrópicas do modelo foi elaborado um programa capaz inserir os volumes do poluente SO2 de forma horária expelidos pela chaminé, de acordo com as taxas de emissão medidos diretamente na fonte. O programa representou a emissão do poluente no ponto de grade correspondente a localização e a altura acima da superfície da chaminé da fonte. As simulações foram configuradas com os seguintes esquemas de parametrização: para microfísica de nuvens foi utilizado o Goddard Cumulus Ensemble; os esquemas de radiação de onda longa e curta foram o Goddard e o Rapid Radiative Transfer Model para modelos de circulação geral da atmosfera (MCGA); para a parametrização de cumulus o esquema utilizado foi o Grell 3D Ensemble Scheme; e para os esquemas de camada superficial e camada limite planetária foram utilizados os da teoria da similaridade do Fifth-Generation National Center for Atmospheric Research/Penn State Mesoscale Model (MM5) e o Yonsey University, respectivamente. A escolha desta combinação de esquemas foi definida a partir de um estudo inicial da sensibilidade do modelo à mudança das parametrizações. Os resultados dos experimentos numéricos alterando a topografia foram validados a partir dos dados de monitoramento das estações meteorológica e da qualidade do ar pertencentes à empresa responsável pelo empreendimento associado à fonte. Foi observado que as simulações com os dados SRTM expressaram o terreno da região de estudo mais próximo à realidade, representando o aspecto heterogêneo do relevo, ressaltando os picos e os vales. Os resultados das validações meteorológicas utilizando os dados topográficos indicaram melhoras nas simulações das variáveis meteorológicas: temperatura, umidade relativa, velocidade do vento e precipitação. Os experimentos com os dados topográficos GTOPO e SRTM no modelo WRF/Chem, configurado com as emissões horárias da fonte de Candiota, reproduziram o comportamento dos ventos para transporte de SO2 até as estações de monitoramento conforme os dados observados. Porém foram identificados padrões diferentes na representação das concentrações do poluente entre as duas simulações do modelo, associados aos escoamentos dos ventos representados pelos experimentos. A resolução da topografia afetou na simulação de SO2 devido ao aumento da forçante superficial induzida pelo terreno. Este aumento na forçante, influenciou a advecção da pluma de SO2, resultando em diferentes padrões das concentrações de SO2 no ponto de grade correspondente às estações de monitoramento. Contudo, os resultados das simulações das concentrações de SO2, tanto de forma horária quanto na abordagem das médias diárias, não indicaram uma relação linear entre a utilização de dados em alta resolução e a melhora na representação do SO2 pelo modelo WRF/Chem. / The objective of this work was to analyze the impact of the higher resolution topographic data sets in the simulations of the Sulfur dioxide (SO2) concentrations emitted by a source located Southern Brazil. Two simulations were performed applying the Weather Research and Forecasting model coupled with Chemistry – WRF/Chem, configured with two representations of the terrain with different spatial resolutions. The standard data of the model with the best resolution (approximately 1 km), Global 30 Arc-Second Elevation (GTOPO), and was inserted in the model databases the high-resolution (30 meters) terrain information of the Radar Shuttle Topography Mission (SRTM). For the anthropic emissions of the model, a program was developed capable of inserting the hourly SO2 pollutant volumes expelled by the chimney, according to the emission rates measured directly at the source. The program inserted these emissions into the grid point corresponding to the location and height above the surface of the emission source. The simulations were configured with the following parameterization schemes: for cloud microphysics Goddard Cumulus Ensemble; for the long and short wave radiation treatment it was used the Goddard and the Rapid Radiative Transfer Model for general circulation models; for the cumulus parameterization the scheme it was used the Grell 3D Ensemble Scheme; and for the surface layer and planetary boundary layer schemes, the similarity theory of the Fifth-Generation National Center for Atmospheric Research/Penn State Mesoscale Model (MM5) and the Yonsey University, respectively. The choice of this combination of schemes was defined from an initial study of the sensitivity of the model to the change of parametrizations. The results of the numerical experiments altering the topography were validated from the monitoring data of the meteorological stations and the air quality belonging to the company responsible for the enterprise associated to the source. It was observed that the simulations with the SRTM data expressed the terrain of the region of study closest to reality, representing the heterogeneous aspect of the terrain, highlighting the peaks and valleys. The results of the meteorological validations using the new topographic data indicated an improvement in the simulations of the meteorological variables: temperature, relative humidity, wind speed and precipitation. The experiments with the GTOPO and SRTM topographic data in WRF/Chem model, configured with the hourly emissions of the Candiota source, reproduced the winds behavior that transported the SO2 to the monitoring stations according to the observed data. However, different patterns were identified in the pollutant concentrations between the two simulations of the model, associated to the wind flows represented by the experiments. The topography resolution affected in the simulation of SO2 due to the increase of the surface forcing induced by the terrain. This increase in the forcing influenced the advection of the SO2 plume, resulting in different patterns of SO2 concentrations at the grid point corresponding to the monitoring stations. However, the results of simulations of SO2 concentrations, both hourly and in the approach of daily averages, did not indicate a linear relationship between the use of high resolution data and the improvement in the representation of SO2 by WRF/Chem model.

Abstract : This is a study concerning comparisons between the Dubovik Aerosol optical depth (AOD) retrievals from AEROCAN (ARONET) stations and AOD estimates from simulations provided by a chemical transport model (GEOS-Chem : Goddard Earth Observing System Chemistry). The AOD products associated with the Dubovik product are divided into total, fine and coarse mode components. The retrieval period is from January 2009 to January 2013 for 5 Arctic stations (Barrow, Alaska; Resolute Bay, Nunavut; 0PAL and PEARL (Eureka), Nunavut; and Thule, Greenland). We also employed AOD retrievals from 10 other mid-latitude Canadian stations for comparisons with the Arctic stations. The results of our investigation were submitted to Atmosphere-Ocean. To briefly summarize those results, the model generally but not always tended to underestimate the (monthly) averaged AOD and its components. We found that the subdivision into fine and coarse mode components could provide unique signatures of particular events (Asian dust) and that the means of characterizing the statistics (log-normal frequency distributions versus normal distributions) was an attribute that was common to both the retrievals and the model. / Résumé : Cette étude compare des épaisseurs optiques d’aérosols (AOD) à 5 stations arctiques d’AEROCAN (AERONET), obtenues d’une part à l’aide de l’algorithme d'inversion de Dubovik appliqué à des mesures in situ, et d’autre part du modèle de transport chimique (GEOS-Chem : Goddard Earth Observing Système Chemistry). Les produits d’AOD associés à l’algorithme d’inversion sont divisés en composantes totales, fines et grossières. Pour chacune des 5 stations (Barrow, Alaska, Resolute Bay, au Nunavut, 0PAL et PEARL (Eureka), Nunavut, et Thulé, au Groenland), la période de récupération est de janvier 2009 à janvier 2013. Nous avons également utilisé les mesureurs d’AOD de dix autres stations canadiennes de latitudes moyennes, à des fins de comparaison. Les résultats de l’étude ont été soumis à la revue Atmosphere-Ocean. Pour résumer brièvement ces résultats, le modèle a généralement, mais pas toujours, eu tendance à sous-estimer l'AOD moyenne et de ses composantes. Nous avons constaté que la subdivision en composantes fine et grossière pourrait fournir des signatures uniques d'événements particuliers (poussière asiatique) et que les moyens de caractériser des statistiques (les distributions de fréquence log-normale versus les distributions normales) était un attribut qui était commun aux deux les mesureurs et le modèle.

O objetivo deste trabalho foi o analisar o impacto da resolução dos conjuntos de dados topográficos nas simulações das concentrações de dióxido de enxofre (SO2) emitido por uma fonte localizada no Sul do Brasil. Para isso foram realizadas duas simulações aplicando o modelo regional Weather Research and Forecasting acoplado com a química (WRF/Chem), configurado com duas representações do terreno de diferentes resoluções espaciais. Foram utilizados os dados padrão do modelo com melhor resolução, Global 30 Arc-Second Elevation (GTOPO), com aproximadamente 1 km, e inserido no bancos de dados do modelo as informações de terreno em alta-resolução do Radar Shuttle Topography Mission (SRTM) (30 metros). Para as emissões antrópicas do modelo foi elaborado um programa capaz inserir os volumes do poluente SO2 de forma horária expelidos pela chaminé, de acordo com as taxas de emissão medidos diretamente na fonte. O programa representou a emissão do poluente no ponto de grade correspondente a localização e a altura acima da superfície da chaminé da fonte. As simulações foram configuradas com os seguintes esquemas de parametrização: para microfísica de nuvens foi utilizado o Goddard Cumulus Ensemble; os esquemas de radiação de onda longa e curta foram o Goddard e o Rapid Radiative Transfer Model para modelos de circulação geral da atmosfera (MCGA); para a parametrização de cumulus o esquema utilizado foi o Grell 3D Ensemble Scheme; e para os esquemas de camada superficial e camada limite planetária foram utilizados os da teoria da similaridade do Fifth-Generation National Center for Atmospheric Research/Penn State Mesoscale Model (MM5) e o Yonsey University, respectivamente. A escolha desta combinação de esquemas foi definida a partir de um estudo inicial da sensibilidade do modelo à mudança das parametrizações. Os resultados dos experimentos numéricos alterando a topografia foram validados a partir dos dados de monitoramento das estações meteorológica e da qualidade do ar pertencentes à empresa responsável pelo empreendimento associado à fonte. Foi observado que as simulações com os dados SRTM expressaram o terreno da região de estudo mais próximo à realidade, representando o aspecto heterogêneo do relevo, ressaltando os picos e os vales. Os resultados das validações meteorológicas utilizando os dados topográficos indicaram melhoras nas simulações das variáveis meteorológicas: temperatura, umidade relativa, velocidade do vento e precipitação. Os experimentos com os dados topográficos GTOPO e SRTM no modelo WRF/Chem, configurado com as emissões horárias da fonte de Candiota, reproduziram o comportamento dos ventos para transporte de SO2 até as estações de monitoramento conforme os dados observados. Porém foram identificados padrões diferentes na representação das concentrações do poluente entre as duas simulações do modelo, associados aos escoamentos dos ventos representados pelos experimentos. A resolução da topografia afetou na simulação de SO2 devido ao aumento da forçante superficial induzida pelo terreno. Este aumento na forçante, influenciou a advecção da pluma de SO2, resultando em diferentes padrões das concentrações de SO2 no ponto de grade correspondente às estações de monitoramento. Contudo, os resultados das simulações das concentrações de SO2, tanto de forma horária quanto na abordagem das médias diárias, não indicaram uma relação linear entre a utilização de dados em alta resolução e a melhora na representação do SO2 pelo modelo WRF/Chem. / The objective of this work was to analyze the impact of the higher resolution topographic data sets in the simulations of the Sulfur dioxide (SO2) concentrations emitted by a source located Southern Brazil. Two simulations were performed applying the Weather Research and Forecasting model coupled with Chemistry – WRF/Chem, configured with two representations of the terrain with different spatial resolutions. The standard data of the model with the best resolution (approximately 1 km), Global 30 Arc-Second Elevation (GTOPO), and was inserted in the model databases the high-resolution (30 meters) terrain information of the Radar Shuttle Topography Mission (SRTM). For the anthropic emissions of the model, a program was developed capable of inserting the hourly SO2 pollutant volumes expelled by the chimney, according to the emission rates measured directly at the source. The program inserted these emissions into the grid point corresponding to the location and height above the surface of the emission source. The simulations were configured with the following parameterization schemes: for cloud microphysics Goddard Cumulus Ensemble; for the long and short wave radiation treatment it was used the Goddard and the Rapid Radiative Transfer Model for general circulation models; for the cumulus parameterization the scheme it was used the Grell 3D Ensemble Scheme; and for the surface layer and planetary boundary layer schemes, the similarity theory of the Fifth-Generation National Center for Atmospheric Research/Penn State Mesoscale Model (MM5) and the Yonsey University, respectively. The choice of this combination of schemes was defined from an initial study of the sensitivity of the model to the change of parametrizations. The results of the numerical experiments altering the topography were validated from the monitoring data of the meteorological stations and the air quality belonging to the company responsible for the enterprise associated to the source. It was observed that the simulations with the SRTM data expressed the terrain of the region of study closest to reality, representing the heterogeneous aspect of the terrain, highlighting the peaks and valleys. The results of the meteorological validations using the new topographic data indicated an improvement in the simulations of the meteorological variables: temperature, relative humidity, wind speed and precipitation. The experiments with the GTOPO and SRTM topographic data in WRF/Chem model, configured with the hourly emissions of the Candiota source, reproduced the winds behavior that transported the SO2 to the monitoring stations according to the observed data. However, different patterns were identified in the pollutant concentrations between the two simulations of the model, associated to the wind flows represented by the experiments. The topography resolution affected in the simulation of SO2 due to the increase of the surface forcing induced by the terrain. This increase in the forcing influenced the advection of the SO2 plume, resulting in different patterns of SO2 concentrations at the grid point corresponding to the monitoring stations. However, the results of simulations of SO2 concentrations, both hourly and in the approach of daily averages, did not indicate a linear relationship between the use of high resolution data and the improvement in the representation of SO2 by WRF/Chem model.

Atmospheric aerosol particles play an important role in global climate change, via direct and indirect radiative forcing. Elemental carbon (EC) and nitrate are important contributors to anthropogenic aerosol radiative forcing over Europe, since they strongly absorb and/or scatter solar radiation, respectively. However, the evaluation of their climate effects remains highly uncertain. Improvements on the simulation of particle number/mass size distribution (PSD) in modelling will help us to refine model assessments of climate change. The simulations were performed over Europe with a fully online-coupled regional air quality model (WRF-Chem) for the time period of September 10-20th, 2013. Measurements in the HOPE-Melpitz campaign and other datasets in Europe were adopted to evaluate the model uncertainties. The meteorological conditions were well reproduced by the simulations. However, a remarkable overestimation of coarse mode PSD was found in the simulations. The overestimation was mainly contributed by EC, sodium nitrate and sea salt (SSA), stemming from the inadequate emission of EC and SSA. The EC inventory overestimates EC point sources in Germany and the fractions of coarse mode EC emissions in Eastern Europe and Russia. Allocating too much EC emission into the coarse mode could shorten EC lifetime and reduce its long-range transport, thus partly (~20-40%) explaining the underestimation of EC in Germany, when air masses came from eastern direction in previous studies. Furthermore, WRF-Chem overestimated coarse mode SSA mass concentrations by factors of about 8-20 over northwestern and central Europe in this study, due to the shortcoming of its emission scheme. This could facilitate the coarse mode sodium nitrate formation and lead to ~140% overestimation of coarse mode nitrate. Under such circumstances, nitric acid was exhausted, and fine mode ammonium nitrate formation was inhibited. The overestimated SSA shaped the PSD of nitrate towards larger sizes, which might influence the optical properties, lifetime and climate effect of nitrate accordingly. A transport mechanism would broaden the influence of SSA on nitrate PSD to central Europe, where a considerable amount of nitrate precursors and ammonium nitrate is present.:Table of Contents List of Figures List of Tables Abbreviations 1. Introduction 1.1 Particle size distribution 1.2 Elemental carbon particle size distribution simulation 1.3 Chemical pathways for particulate nitrate 1.4 Influence of sea salt on nitrate particle mass size distribution 1.5 Objectives 2. Methodology 2.1. WRF-Chem model 2.1.1. General description 2.1.2. Model configuration 2.1.3 Anthropogenic source emissions 2.1.4 Natural source emissions 2.2 HOPE-Melpitz campaign 2.3 GUAN network over Germany 2.4 Other datasets 3. Results and Discussion 3.1 First publication 3.1.1 Evaluation of the size segregation of elemental carbon (EC) emission in Europe: influence on the simulation of EC long-range transportation 3.1.2 Supporting information 3.2 Second publication 3.2.1 Sea salt emission, transport and influence on size-segregated nitrate simulation: a case study in northwestern Europe by WRF-Chem 3.2.2 Supporting information 4. Summary and Conclusions 5. Outlook Appendix A Bibliography Acknowledgements