Abstract: Smoke particles ejected into the atmosphere from biomass burning can modify the atmospheric composition around and even far from the sources. In late winter and early spring, biomass burning emissions from inland regions can be efficiently transported to urban areas in southeastern South America, thus affecting air quality in those areas. In this study, the Weather Research and Forecasting with Chemistry model was applied in order to investigate the impact of biomass burning sources on aerosol loadings and properties over the São Paulo Metropolitan Area (SPMA), in southeastern Brazil, during the period from 19 August to 3 September 2014. The model performance was evaluated using available aerosol measurements from the Narrowing the Uncertainties on Aerosol and Climate Change in São Paulo State project. The combined application of aerosol data and Weather Research and Forecasting with Chemistry simulations made it possible to represent some of the most important aerosol properties, such as particle number concentration and cloud condensation nuclei activation, in addition to evaluation of the impact of biomass burning by analyzing a 5‐day transport event, from 22 to 26 August 2014. During this transport event, differences in the average predicted PM2.5 concentration reached 15 μg/m3 (peaking at 20 μg/m3 during the nighttime hours) over the SPMA, compared with 35 μg/m3 over inland areas northwest and north of the SPMA. Biomass burning accounted for up to 20% of the baseline particle number concentration‐ and cloud condensation nuclei‐weighted relative differences over the SPMA (2,300 and 1,400 cm−3, respectively).

Palavras-Chave: aerosols; aerosol wastes; atmospheric circulation; air pollution monitoring; smoke detectors; climatic change; biofuels; aerosol monitoring; solar radiation; brazil; meteorology; evaluation

Abstract: On 22 April 2015, the Calbuco volcano in Chile (Lat: 41.33 S, Long: 72.62 W) erupted after 43 years of inactivity followed by a great amount of aerosol injection into the atmosphere. The pyroclastic material dispersed into the atmosphere posed a potential threat to aviation traffic and air quality over affected a large area. The plumes and debris spread from its location to Patagonian and Pampean regions, reaching the Atlantic and Pacific Oceans and neighboring countries, such as Argentina, Brazil and Uruguay, driven by the westerly winds at these latitudes. The presence of volcanic aerosol layers could be identified promptly at the proximities of Calbuco and afterwards by remote sensing using satellites and lidars in the path of the dispersed aerosols. The Cloud-Aerosol Lidar and Pathfinder Satellite Observations (CALIPSO), Moderate Resolution Imaging Spectroradiometer (MODIS) on board of AQUA/TERRA satellites and Ozone Mapping and Profiler Suite (OMPS) on board of Suomi National Polar-orbiting Partnership (Suomi NPP) satellite were the space platforms used to track the injected layers and a multi-channel lidar system from Latin America Lidar Network (LALINET) SPU Lidar station in South America allowed us to get the spatial and temporal distribution of Calbuco ashes after its occurrence. The SPU lidar stations co-located Aerosol Robotic Network (AERONET) sunphotometers to help in the optical characterization. Here, we present the volcanic layer transported over São Paulo area and the detection of aerosol plume between 18 and 20 km. The path traveled by the volcanic aerosol to reach the Metropolitan Area of São Paulo (MASP) was tracked by CALIPSO and the aerosol optical and geometrical properties were retrieved at some points to monitor the plume evolution. Total attenuated backscatter profile at 532 nm obtained by CALIPSO revealed the height range extension of the aerosol plume between 18 and 20 km and are in agreement with SPU lidar range corrected signal at 532 nm. The daily evolution of Aerosol Optical Depth (AOD) at 532 and 355 nm, retrieved from AERONET sunphotometer, showed a substantial increasing on 27 April, the day of the volcanic plume detection at Metropolitan Area of São Paulo (MASP), achieving values of 0.33 0.16 and 0.22 0.09 at 355 and 532 nm, respectively. AERONET aerosol size distribution was dominated by fine mode aerosol over coarse mode, especially on 27 and 28 April. The space and time coincident aerosol extinction profiles from SPU lidar station and OMPS LP from the Calbuco eruption conducted on 27 April agreed on the double layer structure. The main objective of this study was the application of the transmittance method, using the Platt formalism, to calculate the optical and physical properties of volcanic plume, i.e., aerosol bottom and top altitude, the aerosol optical depth and lidar ratio. The aerosol plume was detected between 18 and 19.3 km, with AOD value of 0.159 at 532 nm and Ånsgtröm exponent of 0.61 0.58. The lidar ratio retrieved was 76 27 sr and 63 21 sr at 532 and 355 nm, respectively. Considering the values of these parameters, the Calbuco volcanic aerosol layers could be classified as sulfates with some ash type.

Palavras-Chave: volcanoes; ashes; aerosols; boundary layers; atmospheric circulation; optical radar; south america; air quality

Abstract: Biomass burning is a significant source of trace gases and aerosols to the atmosphere, and the evolution of these species depends acutely on where they are injected into the atmosphere. GEOS-Chem is a chemical transport model driven by assimilated meteorological data that is used to probe a variety of scientific questions related to atmospheric composition, including the role of biomass burning. This paper presents the development and implementation of a new global biomass burning emissions injection scheme in the GEOS-Chem model. The new injection scheme is based on monthly gridded Multi-angle Imaging SpectroRadiometer (MISR) global plume-height stereoscopic observations in 2008. To provide specific examples of the impact of the model updates, we compare the output from simulations with and without the new MISR-based injection height scheme to several sets of observations from regions with active fires. Our comparisons with Arctic Research on the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) aircraft observations show that the updated injection height scheme can improve the ability of the model to simulate the vertical distribution of peroxyacetyl nitrate (PAN) and carbon monoxide (CO) over North American boreal regions in summer.We also compare a simulation for October 2010 and 2011 to vertical profiles of CO over the Amazon Basin. When coupled with larger emission factors for CO, a simulation that includes the new injection scheme also better matches selected observations in this region. Finally, the improved injection height improves the simulation of monthly mean surface CO over California during July 2008, a period with large fires.

Palavras-Chave: biofuels; biomass; atmospheric circulation; carbon; emission; amazon river; atmospheric chemistry; meteorology; gases

Abstract: A 12-year analysis, from 2005 to 2016, of atmospheric aerosol optical properties focusing for the first time on Northeast Brazil (NEB) was performed based on four di erent remote sensing datasets: the Moderate Resolution Imaging Spectroradiometer (MODIS), the Aerosol Robotic Network (AERONET), the Cloud-Aerosol LIDAR with Orthogonal Polarization (CALIOP) and a ground-based Lidar from Natal. We evaluated and identified distinct aerosol types, considering Aerosol Optical Depth (AOD) and Angström Exponent (AE). All analyses show that over the NEB, a low aerosol scenario prevails, while there are two distinct seasons of more elevated AOD that occur every year, from August to October and January to March. According to MODIS, AOD values ranges from 0.04 to 0.52 over the region with a mean of 0.20 and occasionally isolated outliers of up to 1.21. Aerosol types were identified as sea spray, biomass burning, and dust aerosols mostly transported from tropical Africa. Three case studies on days with elevated AOD were performed. All cases identified the same aerosol types and modeled HYSPLIT backward trajectories confirmed their source-dependent origins. This analysis is motivated by the implementation of an atmospheric chemistry model with an advanced data assimilation system that will use the observational database over NEB with the model to overcome high uncertainties in the model results induced by still unvalidated emission inventories.

Palavras-Chave: aerosols; aerosol monitoring; optical radar; dusts; datasets; satellites; atmospherics; meteorology; optical properties; brazil; atmospheric circulation

Abstract: Sulfuric acid is a key contributor to new particle formation, though measurements of its gaseous concentrations are difficult to make. Several parameterizations to estimate sulfuric acid exist, all of which were constructed using measurements from the Northern Hemisphere. In this work, we report the first measurements of sulfuric acid from the Amazon basin. These measurements are consistent with concentrations measured in Hyytiälä, Finland, though, unlike Hyytiälä, there is no clear correlation of sulfuric acid with global radiation. There was a minimal difference in sulfuric acid observed between the wet and dry seasons in the Amazon basin. We also test the efficacy of existing proxies to estimate sulfuric acid in this region. Our results suggest that nighttime sulfuric acid production is due to both a stabilized Criegee intermediate pathway and oxidation of SO2 by OH, the latter of which is not currently accounted for in existing proxies. These results also illustrate the drawbacks of the common substitution of radiation for OH concentrations. None of the tested proxies effectively estimate sulfuric acid measurements at night. For estimates at all times of day, a recently published proxy based on data from the boreal forest should be used. If only daytime estimates are needed, several recent proxies that do not include the Criegee pathway are sufficient. More investigation of nighttime sulfuric acid production pathways is necessary to close the gap between measurements and estimates with existing proxies.

Palavras-Chave: sulfuric acid; atmospheric circulation; aerosols; hydroxyl radicals; amazon river