Over the last decade we have witnessed a rapid, so far unexplained, increase in the emission of methane to the atmosphere and this increase could lead to an acceleration of the ongoing climate ...changes. The increase is likely to originate from agriculture, but oil and gas production as well as wetlands are also under suspicion. The best way to quantify the emission of methane and other greenhouse gasses to our atmosphere is by using space based remote sensing. Here, we analyse 3 years of measurements of the column-averaged dry-air mole fraction of methane from the Tropospheric Monitoring Instrument on Sentinel-5P obtained with two different retrieval methods in order to evaluate the dependency on geographic, land cover type and season. The land cover types were obtained from the Moderate Resolution Imaging Spectroradiometer aboard the Terra and Aqua satellites and from the World Cover data product using observations from the Copernicus Sentinel-1 and Sentinel-2 missions. The analysis reveals that while the highest methane concentrations are generally found over croplands, the lowest are generally found over shrublands, which is in agreement with expectations. It is more surprising that the analysis also reveals lower than average methane concentrations over wetlands as wetlands are generally thought to be a major source of methane emission. Until this discrepancy is resolved the methane concentration over wetlands from the Tropospheric Monitoring Instrument on Sentinel-5P should be handled with caution. It is also found that the annual methane cycle, as seen in the measured methane concentrations, for croplands, shrublands and savannas is delayed in Africa compared to Asia.
The Green Ocean Amazon experiment – GoAmazon 2014–2015 – explored the interactions between natural biogenic forest emissions from central Amazonia and urban air pollution from Manaus. Previous ...GoAmazon 2014–2015 studies showed that nitrogen oxide (NOx = NO + NO2) and sulfur oxide (SOx) emissions from Manaus strongly interact with biogenic volatile organic compounds (BVOCs), affecting secondary organic aerosol (SOA) formation. In previous studies, ground-based and aircraft measurements provided evidence of SOA formation and strong changes in aerosol composition and properties. Aerosol optical properties also evolve, and their impacts on the Amazonian ecosystem can be significant. As particles age, some processes, such as SOA production, black carbon (BC) deposition, particle growth and the BC lensing effect change the aerosol optical properties, affecting the solar radiation flux at the surface. This study analyzes data and models SOA formation using the Weather Research and Forecasting with Chemistry (WRF-Chem) model to assess the spatial variability in aerosol optical properties as the Manaus plumes interact with the natural atmosphere. The following aerosol optical properties are investigated: single scattering albedo (SSA), asymmetry parameter (gaer), absorption Ångström exponent (AAE) and scattering Ångström exponent (SAE). These simulations were validated using ground-based measurements at three experimental sites, namely the Amazon Tall Tower Observatory – ATTO (T0a), downtown Manaus (T1), Tiwa Hotel (T2) and Manacapuru (T3), as well as the U.S. Department of Energy (DOE) Gulfstream 1 (G-1) aircraft flights. WRF-Chem simulations were performed over 7 d during March 2014. Results show a mean biogenic SOA (BSOA) mass enrichment of 512 % at the T1 site, 450 % in regions downwind of Manaus, such as the T3 site, and 850 % in areas north of the T3 site in simulations with anthropogenic emissions. The SOA formation is rather fast, with about 80 % of the SOA mass produced in 3–4 h. Comparing the plume from simulations with and without anthropogenic emissions, SSA shows a downwind reduction of approximately 10 %, 11 % and 6 % at the T1, T2 and T3 sites, respectively. Other regions, such as those further downwind of the T3 site, are also affected. The gaer values increased from 0.62 to 0.74 at the T1 site and from 0.67 to 0.72 at the T3 site when anthropogenic emissions are active. During the Manaus plume-aging process, a plume tracking analysis shows an increase in SSA from 0.91 close to Manaus to 0.98 160 km downwind of Manaus as a result of SOA production and BC deposition.
Methane is the second-most important greenhouse gas after carbon dioxide and accounts for around 10 % of total European Union greenhouse gas emissions. Given that the atmospheric methane budget over ...a region depends on its terrestrial and aquatic methane sources, inverse modelling techniques appear as powerful tools for identifying critical areas that can later be submitted to emission mitigation strategies. In this regard, an inverse modelling system of methane emissions for Europe is being implemented based on the Weather Research and Forecasting (WRF) model: the Aarhus University Methane Inversion Algorithm (AUMIA) v1.0. The forward modelling component of AUMIA consists of the WRF model coupled to a multipurpose global database of methane anthropogenic emissions. To assure transport consistency during the inversion process, the backward modelling component will be based on the WRF model coupled to a Lagrangian particle dispersion module. A description of the modelling tools, input data sets, and 1-year forward modelling evaluation from 1 April 2018 to 31 March 2019 is provided in this paper. The a posteriori methane emission estimates, including a more focused inverse modelling for Denmark, will be provided in a second paper. A good general agreement is found between the modelling results and observations based on the TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor satellite. Model-observation discrepancies for the summer peak season are in line with previous studies conducted over urban areas in central Europe, with relative differences between simulated concentrations and observational data in this study ranging from 1 % to 2 %. Domain-wide correlation coefficients and root-mean-square errors for summer months ranged from 0.4 to 0.5 and from 27 to 30 ppb, respectively. On the other hand, model-observation discrepancies for winter months show a significant overestimation of anthropogenic emissions over the study region, with relative differences ranging from 2 % to 3 %. Domain-wide correlation coefficients and root-mean-square errors in this case ranged from 0.1 to 0.4 and from 33 to 50 ppb, respectively, indicating that a more refined inverse analysis assessment will be required for this season. According to modelling results, the methane enhancement above the background concentrations came almost entirely from anthropogenic sources; however, these sources contributed with only up to 2 % to the methane total-column concentration. Contributions from natural sources (wetlands and termites) and biomass burning were not relevant during the study period. The results found in this study contribute with a new model evaluation of methane concentrations over Europe and demonstrate a huge potential for methane inverse modelling using improved TROPOMI products in large-scale applications.
The Amazon rainforest suffers increasing pressure from anthropogenic activities. A key aspect not fully understood is how anthropogenic atmospheric emissions within the basin interact with biogenic ...emissions and impact the forest’s atmosphere and biosphere. We combine a high-resolution atmospheric chemical transport model with an improved emissions inventory and in-situ measurements to investigate a surprisingly high concentration of ozone (O3) and secondary organic aerosol (SOA) 150–200 km downwind of Manaus city in an otherwise pristine forested region. We show that atmospheric dynamics and photochemistry determine a gross production of secondary pollutants seen in the simulation. After sunrise, the erosion of the nocturnal boundary layer mixes natural forest emissions, rich in biogenic volatile organic compounds, with a lofted pollution layer transported overnight, rich in nitrogen oxides and formaldehyde. As a result, O3 and SOA concentrations greater than ∼47 ppbv and 1.8 μg m–3, respectively, were found, with maximum concentrations occurring at 2 pm LT, 150–200 km downwind of Manaus city. These high concentrations affect a large primary forested area of about 11,250 km2. These oxidative areas are under a NOx-limited regime so that changes in NOx emissions from Manaus have a significant impact on O3 and SOA production.
Methane is the second-most important greenhouse gas after carbon dioxide and accounts for around 10 % of total European Union greenhouse gas emissions. Given that the atmospheric methane budget over ...a region depends on its terrestrial and aquatic methane sources, inverse modelling techniques appear as powerful tools for identifying critical areas that can later be submitted to emission mitigation strategies. In this regard, an inverse modelling system of methane emissions for Europe is being implemented based on the Weather Research and Forecasting (WRF) model: the Aarhus University Methane Inversion Algorithm (AUMIA) v1.0. The forward modelling component of AUMIA consists of the WRF model coupled to a multipurpose global database of methane anthropogenic emissions. To assure transport consistency during the inversion process, the backward modelling component will be based on the WRF model coupled to a Lagrangian particle dispersion module. A description of the modelling tools, input data sets, and 1-year forward modelling evaluation from 1 April 2018 to 31 March 2019 is provided in this paper. The a posteriori methane emission estimates, including a more focused inverse modelling for Denmark, will be provided in a second paper. A good general agreement is found between the modelling results and observations based on the TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor satellite. Model–observation discrepancies for the summer peak season are in line with previous studies conducted over urban areas in central Europe, with relative differences between simulated concentrations and observational data in this study ranging from 1 % to 2 %. Domain-wide correlation coefficients and root-mean-square errors for summer months ranged from 0.4 to 0.5 and from 27 to 30 ppb, respectively. On the other hand, model–observation discrepancies for winter months show a significant overestimation of anthropogenic emissions over the study region, with relative differences ranging from 2 % to 3 %. Domain-wide correlation coefficients and root-mean-square errors in this case ranged from 0.1 to 0.4 and from 33 to 50 ppb, respectively, indicating that a more refined inverse analysis assessment will be required for this season. According to modelling results, the methane enhancement above the background concentrations came almost entirely from anthropogenic sources; however, these sources contributed with only up to 2 % to the methane total-column concentration. Contributions from natural sources (wetlands and termites) and biomass burning were not relevant during the study period. The results found in this study contribute with a new model evaluation of methane concentrations over Europe and demonstrate a huge potential for methane inverse modelling using improved TROPOMI products in large-scale applications.
Methane is the second-most important greenhouse gas after carbon dioxide and accounts for around 10 % of total European Union greenhouse gas emissions. Given that the atmospheric methane budget over ...a region depends on its terrestrial and aquatic methane sources, inverse modelling techniques appear as powerful tools for identifying critical areas that can later be submitted to emission mitigation strategies. In this regard, an inverse modelling system of methane emissions for Europe is being implemented based on the Weather Research and Forecasting (WRF) model: the Aarhus University Methane Inversion Algorithm (AUMIA) v1.0. The forward modelling component of AUMIA consists of the WRF model coupled to a multipurpose global database of methane anthropogenic emissions. To assure transport consistency during the inversion process, the backward modelling component will be based on the WRF model coupled to a Lagrangian particle dispersion module. A description of the modelling tools, input data sets, and 1-year forward modelling evaluation from 1 April 2018 to 31 March 2019 is provided in this paper. The a posteriori methane emission estimates, including a more focused inverse modelling for Denmark, will be provided in a second paper. A good general agreement is found between the modelling results and observations based on the TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor satellite. Model–observation discrepancies for the summer peak season are in line with previous studies conducted over urban areas in central Europe, with relative differences between simulated concentrations and observational data in this study ranging from 1 % to 2 %. Domain-wide correlation coefficients and root-mean-square errors for summer months ranged from 0.4 to 0.5 and from 27 to 30 ppb, respectively. On the other hand, model–observation discrepancies for winter months show a significant overestimation of anthropogenic emissions over the study region, with relative differences ranging from 2 % to 3 %. Domain-wide correlation coefficients and root-mean-square errors in this case ranged from 0.1 to 0.4 and from 33 to 50 ppb, respectively, indicating that a more refined inverse analysis assessment will be required for this season. According to modelling results, the methane enhancement above the background concentrations came almost entirely from anthropogenic sources; however, these sources contributed with only up to 2 % to the methane total-column concentration. Contributions from natural sources (wetlands and termites) and biomass burning were not relevant during the study period. The results found in this study contribute with a new model evaluation of methane concentrations over Europe and demonstrate a huge potential for methane inverse modelling using improved TROPOMI products in large-scale applications.
A comprehensive Weather Research and Forecasting with Chemistry (WRF-Chem) model evaluation is conducted using ground-based and total column observational data from air quality stations and satellite ...retrievals. Fine particles (PM2.5; ≤ 2.5 μm in aerodynamic diameter), nitrogen oxides (NOx, NO + NO2), carbon monoxide (CO), tropospheric ozone (O3) concentrations and AOD values over southeastern Brazil were analyzed to assess the model's capability in reproducing atmospheric observation. The model simulations were performed over simple one domain at grid resolution of 10 km over southeastern Brazil. This spatial resolution was chosen due to a previous evaluation between five MODIS AOD products with AERONET estimates, resulting in Dark Target at 10 km of spatial resolution the best product to represent the AOD values over our study domain. Model input emissions comprise vehicular emissions derived from a bottom-up emission model, as well as on-line calculations of biogenic and fire emission rates. Given that the atmospheric state affects air pollution dispersion, a model evaluation on the meteorological conditions was carried out to better evaluate the model performance in reproducing the pollutant concentrations. Good agreement between model simulations and observations for air temperature and relative humidity at 2 m height was found, with correlation coefficients higher than 0.85 in most periods. Expected benchmarks for wind speed and direction at 10 m height were also found in this analysis, though with larger uncertainties. Underestimation occurred for daily accumulated precipitation due to the limitations of the cloud microphysics scheme or cumulus parameterization. Model simulations of PM2.5, NOx, CO and O3 agreed well with ground-based observations in terms of temporal variations and trends, with model-observation discrepancies due to uncertainties in the emission inventories. O3 was the better simulated pollutant in terms of temporal variability, with the characteristic large and small amplitudes observed over urban and rural areas being well represented by the model. High O3 concentrations were observed at the Botucatu station, due to transport of pollutants generated in the Metropolitan Area of São Paulo, and were also represented by the model, indicating the need of more active air quality monitoring stations over inland regions in southeastern Brazil. Moderate and high correlation coefficients (ranging 0.46–0.81) were found for tropospheric NO2 VCD and CO column, and AOD at 550 nm due to uncertainties in the emission inventories and aerosol model simplifications. Both the model and satellite captured higher values in similar regions over our study domain. This work represents a first effort, in southeastern Brazil, that combines numerical modeling, remote sensing and ground-based stations to analyze and understand the impact exerted by the emissions of urban pollution over surrounding areas. A more in-depth analysis of the impact of emissions transport to inland regions from urban areas in southeastern Brazil will be discussed in the second part of this work.
•Six-years of validation between AOD MODIS and AERONET over southeastern Brazil.•Local vehicular emissions inventory in four-months high-resolution WRF-Chem modeling over southeastern Brazil.•The WRF-Chem model correlated well with the ground-based and atmospheric column measurements.
Aerosol particles from forest fire events in the Amazon can be effectively transported to urban areas in southeastern South America, thus affecting the air quality over those regions. A combination ...of observational data and a comprehensive air quality modeling system capable of anticipating acute air pollution episodes is therefore required. A new predictive framework for Amazon forest fire smoke dispersion over South America has been developed based on the Weather Research and Forecasting with Chemistry community (WRF-Chem) model. Two experiments of 48-h simulations over South America were performed by using this system at 20-km horizontal resolution, on a daily basis, during August and September of 2018 and 2019. The experiment in 2019 included the very strong 3-week forest fire event, when the São Paulo metropolitan area, located in southeastern South America, was plunged into darkness on August 19. The model results were satisfactorily compared against satellite-based data products and in situ measurements collected from air quality monitoring sites. The system is executed daily immediately after the CPTEC Satellite Division releases the latest active fire locations data and provides 48-h forecasts of regional distributions of chemical species such as CO, PM2.5, and O3. The new modeling system will be used as a benchmark within the framework of the Chemistry of the Atmosphere–Field Experiment in Brazil (CAFE-Brazil) project, which will take place in 2022 over the Amazon.
Hailstorms develop over the La Plata Basin, in south-eastern South America, more often during later winter and early austral spring, between September and October. These systems have significant ...socioeconomic impacts over the region. Thus, a better understanding of how atmospheric drivers modulate the formation of hailstorms is important to improve the forecast of such phenomena. In this study, we selected a hailstorm event observed over the eastern La Plata Basin during 14–15 July 2016 to evaluate the performance of the Brazilian developments on the Regional Atmospheric Modelling System (BRAMS) model. The ability of the model in simulating cloud microphysical properties was evaluated by comparing simulations driven by different global forcings against in situ and remote sensing observations. The model results showed good skill in capturing the basic characteristics of the thunderstorm, particularly in terms of the spatial distribution of hydrometeors. The simulated spatial distribution of hail covers locations where hail fall was reported. The BRAMS simulations suggest that, despite relatively low values of the convective available potential energy (CAPE) (700–1000 J kg−1), environments with strong 0–8-km bulk shear (60–70 kt, ~30.9–36.0 m s–1) can promote the formation of ice clouds and hail fall over the eastern La Plata Basin. To be more conclusive, however, further research is needed to understand how different combinations of CAPE and shear affect hail formation over the region.
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