scholarly journals Supplementary material to "The vertical distribution of biomass burning pollution over tropical South America from aircraft in situ measurements during SAMBBA"

2018 ◽  
Author(s):  
Eoghan Darbyshire ◽  
William T. Morgan ◽  
James D. Allan ◽  
Dantong Liu ◽  
Michael J. Flynn ◽  
...  
Keyword(s):  
South America ◽  
Vertical Distribution ◽  
Biomass Burning ◽  
In Situ Measurements ◽  
Supplementary Material ◽  
The Vertical Distribution ◽  
Tropical South America

scholarly journals The vertical distribution of biomass burning pollution over tropical South America from aircraft in situ measurements during SAMBBA

2019 ◽  
Vol 19 (9) ◽  
pp. 5771-5790 ◽  
Author(s):  
Eoghan Darbyshire ◽  
William T. Morgan ◽  
James D. Allan ◽  
Dantong Liu ◽  
Michael J. Flynn ◽  
...  
Keyword(s):  
Air Quality ◽  
South America ◽  
Vertical Distribution ◽  
Biomass Burning ◽  
Mixing Layer ◽  
Free Troposphere ◽  
The West ◽  
The Vertical Distribution ◽  
Tropical South America

Abstract. We examine processes driving the vertical distribution of biomass burning pollution following an integrated analysis of over 200 pollutant and meteorological profiles measured in situ during the South AMerican Biomass Burning Analysis (SAMBBA) field experiment. This study will aid future work examining the impact of biomass burning on weather, climate and air quality. During the dry season there were significant contrasts in the composition and vertical distribution of haze between western and eastern regions of tropical South America. Owing to an active or residual convective mixing layer, the aerosol abundance was similar from the surface to ∼1.5 km in the west and ∼3 km in the east. Black carbon mass loadings were double as much in the east (1.7 µg m−3) than the west (0.85 µg m−3), but aerosol scattering coefficients at 550 nm were similar (∼120 Mm−1), as too were CO near-surface concentrations (310–340 ppb). We attribute these contrasts to the more flaming combustion of Cerrado fires in the east and more smouldering combustion of deforestation and pasture fires in the west. Horizontal wind shear was important in inhibiting mixed layer growth and plume rise, in addition to advecting pollutants from the Cerrado regions into the remote tropical forest of central Amazonia. Thin layers above the mixing layer indicate the roles of both plume injection and shallow moist convection in delivering pollution to the lower free troposphere. However, detrainment of large smoke plumes into the upper free troposphere was very infrequently observed. Our results reiterate that thermodynamics control the pollutant vertical distribution and thus point to the need for correct model representation so that the spatial distribution and vertical structure of biomass burning smoke is captured. We observed an increase of aerosol abundance relative to CO with altitude both in the background haze and plume enhancement ratios. It is unlikely associated with thermodynamic partitioning, aerosol deposition or local non-fire sources. We speculate it may be linked to long-range transport from West Africa or fire combustion efficiency coupled to plume injection height. Further enquiry is required to explain the phenomenon and explore impacts on regional climate and air quality.

scholarly journals The vertical distribution of biomass burning pollution over tropical South America from aircraft in situ measurements during SAMBBA

2018 ◽  
Author(s):  
Eoghan Darbyshire ◽  
William T. Morgan ◽  
James D. Allan ◽  
Dantong Liu ◽  
Michael J. Flynn ◽  
...  
Keyword(s):  
South America ◽  
Vertical Distribution ◽  
Biomass Burning ◽  
Mixing Layer ◽  
Thin Layers ◽  
Horizontal Wind ◽  
Free Troposphere ◽  
The West ◽  
The Vertical Distribution ◽  
Tropical South America

Abstract. To reduce the uncertainties in processes driving the vertical distribution of biomass burning pollutants, and thus impacts on regional weather and climate, we present an integrated analysis of vertical profiles of pollutants and meteorological parameters measured on flights during the 2012 South American Biomass Burning Analysis (SAMBBA) field experiment. During the dry season there were significant contrasts in the composition and vertical distribution of haze between western and eastern regions of tropical South America. Owing to an active or residual convective mixing layer, the aerosol burden was similar from the surface to ~ 1.5 km in the west and ~ 3 km in the east. Black carbon mass loadings were double in the east (1.7 µg cm−3) than west (0.85 µg cm−3) but aerosol scattering coefficients at 550 nm were similar (~ 120 Mm−1), as too were CO surface concentrations (310–340 ppb). We attribute these contrasts to the more flaming combustion of Cerrado fires in the east and more smouldering combustion of deforestation and pasture fires in the west. Horizontal wind shear was important in inhibiting mixed layer growth and plume rise, in addition to advecting pollutants from the Cerrado regions into the remote tropical forest of central Amazonia. Optically thin layers above the mixing layer indicates roles for both plume injection and shallow moist convection in delivering pollution to the lower free troposphere. However, detrainment of large smoke plumes into the upper free troposphere was very infrequently observed. Our results reiterate that thermodynamics control the pollutant vertical distribution and thus point to the need for correct model representation so the spatial distribution and vertical structure of biomass burning smoke is captured. Our observations of relatively large concentrations of aerosol aloft and of CO near surface suggest that there is a greater contribution of pollutants from more complete combustion with altitude. Release of appropriate emissions from the initial more flaming and later residual smouldering phases of a fire at appropriate altitudes may be especially important to ensure models can accurately predict aerosol-radiation, aerosol-cloud and air quality impacts.

scholarly journals Transformation and aging of biomass burning carbonaceous aerosol over tropical South America from aircraft in-situ measurements during SAMBBA

2019 ◽  
Author(s):  
William T. Morgan ◽  
James D. Allan ◽  
Stéphane Bauguitte ◽  
Eoghan Darbyshire ◽  
Michael J. Flynn ◽  
...  
Keyword(s):  
South America ◽  
Biomass Burning ◽  
Chemical Properties ◽  
Carbonaceous Aerosol ◽  
Air Masses ◽  
Atmospheric Aging ◽  
Primary Driver ◽  
Tropical South America

Abstract. We present a range of airborne in-situ observations of biomass burning carbonaceous aerosol over tropical South America, including a case study of a large tropical forest wildfire and a series of regional survey flights across the Brazilian Amazon and Cerrado. The study forms part of the South American Biomass Burning Analysis (SAMBBA) Project, which was conducted during September and October 2012. We find limited evidence for net increases in aerosol mass through atmospheric aging combined with substantial changes in the chemical properties of organic aerosol (OA). Oxidation of the OA increases significantly and rapidly on the scale of 2.5–3 hours based on our case study analysis and is consistent with secondary organic aerosol production. The observations of limited net enhancement in OA coupled with such changes in chemical composition, imply that evaporation of OA is also occurring to balance these changes. We observe significant coatings on black carbon particles at source, but with limited changes with aging in both particle core size and coating thickness. We quantify variability in the ratio of OA to carbon monoxide across our study as a key parameter representing both initial fire conditions and an indicator of net aerosol production with atmospheric aging. We observe ratios of 0.075–0.13 μg sm−3 ppbv−1 in the west of our study region over the Amazon tropical forest in air masses less influenced by precipitation and a value of 0.095 μg sm−3 ppbv−1 over the Cerrado environment in the east. Such values are consistent with emission factors used by numerical models to represent biomass burning OA emissions. Black carbon particle core sizes typically range from 250–290 nm, while coating thicknesses range from 40–110 nm in air masses less influenced by precipitation. The primary driver of the variability we observe appears to be related to changes at the initial fire source. A key lesson from our study is that the complex nature of the regional aerosol and its drivers precludes aggregating our observations as a function of atmospheric aging due to the many conflating and competing factors present. Our study explores and quantifies key uncertainties in the evolution of biomass burning aerosol at both nearfield and regional scales. Our results suggest that the initial conditions of the fire are the primary driver of carbonaceous aerosol physical and chemical properties over tropical South America, aside from significant oxidation of OA during atmospheric aging. Such findings imply that uncertainties in the magnitude of the aerosol burden and its impact on weather, climate, health and natural ecosystems most likely lie in quantifying emission sources, alongside atmospheric dispersion, transport and removal rather than chemical enhancements in mass.

scholarly journals Transformation and ageing of biomass burning carbonaceous aerosol over tropical South America from aircraft in situ measurements during SAMBBA

2020 ◽  
Vol 20 (9) ◽  
pp. 5309-5326 ◽  
Author(s):  
William T. Morgan ◽  
James D. Allan ◽  
Stéphane Bauguitte ◽  
Eoghan Darbyshire ◽  
Michael J. Flynn ◽  
...  
Keyword(s):  
South America ◽  
Biomass Burning ◽  
Chemical Properties ◽  
Organic Aerosol ◽  
Carbonaceous Aerosol ◽  
Air Masses ◽  
Primary Driver ◽  
Tropical South America

Abstract. We present a range of airborne in situ observations of biomass burning carbonaceous aerosol over tropical South America, including a case study of a large tropical forest wildfire and a series of regional survey flights across the Brazilian Amazon and Cerrado. The study forms part of the South American Biomass Burning Analysis (SAMBBA) project, which was conducted during September and October 2012. We find limited evidence for net increases in aerosol mass through atmospheric ageing combined with substantial changes in the chemical properties of organic aerosol (OA). Oxidation of the OA increases significantly and rapidly on the scale of 2.5–3 h based on our case study analysis and is consistent with secondary organic aerosol production. The observations of limited net enhancement in OA coupled with such changes in chemical composition imply that evaporation of OA is also occurring to balance these changes. We observe significant coatings on black carbon particles at source, but with limited changes with ageing in both particle core size and coating thickness. We quantify variability in the ratio of OA to carbon monoxide across our study as a key parameter representing both initial fire conditions and an indicator of net aerosol production with atmospheric ageing. We observe ratios of 0.075–0.13 µgsm-3ppbv-1 in the west of our study region over the Amazon tropical forest in air masses less influenced by precipitation and a value of 0.095 µgsm-3ppbv-1 over the Cerrado environment in the east (where sm−3 refers to standard metre cubed). Such values are consistent with emission factors used by numerical models to represent biomass burning OA emissions. Black carbon particle core sizes typically range from mean mass diameters of 250 to 290 nm, while coating thicknesses range from 40 to 110 nm in air masses less influenced by precipitation. The primary driver of the variability we observe appears to be related to changes at the initial fire source. A key lesson from our study is that simply aggregating our observations as a function of atmospheric ageing would have been misleading due to the complex nature of the regional aerosol and its drivers, due to the many conflating and competing factors that are present. Our study explores and quantifies key uncertainties in the evolution of biomass burning aerosol at both near-field and regional scales. Our results suggest that the initial conditions of the fire are the primary driver of carbonaceous aerosol physical and chemical properties over tropical South America, aside from significant oxidation of OA during atmospheric ageing. Such findings imply that uncertainties in the magnitude of the aerosol burden and its impact on weather, climate, health and natural ecosystems most likely lie in quantifying emission sources, alongside atmospheric dispersion, transport and removal rather than chemical enhancements in mass.

scholarly journals Supplementary material to "A single-beam photothermal interferometer for in-situ measurements of aerosol light absorption"

2020 ◽  
Author(s):  
Bradley Visser ◽  
Jannis Röhrbein ◽  
Peter Steigmeier ◽  
Luka Drinovec ◽  
Griša Močnik ◽  
...  
Keyword(s):  
Light Absorption ◽  
In Situ Measurements ◽  
Single Beam ◽  
Supplementary Material

scholarly journals Biomass-burning smoke heights over the Amazon observed from space

2019 ◽  
Vol 19 (3) ◽  
pp. 1685-1702 ◽  
Author(s):  
Laura Gonzalez-Alonso ◽  
Maria Val Martin ◽  
Ralph A. Kahn
Keyword(s):  
Vertical Distribution ◽  
Tropical Forest ◽  
Biomass Burning ◽  
Forest Fires ◽  
Atmospheric Stability ◽  
Free Troposphere ◽  
Smoke Plume ◽  
Smoke Plumes ◽  
Drought Conditions ◽  
The Vertical Distribution

Abstract. We characterise the vertical distribution of biomass-burning emissions across the Amazon during the biomass-burning season (July–November) with an extensive climatology of smoke plumes derived from MISR and MODIS (2005–2012) and CALIOP (2006–2012) observations. Smoke plume heights exhibit substantial variability, spanning a few hundred metres up to 6 km above the terrain. However, the majority of the smoke is located at altitudes below 2.5 km. About 60 % of smoke plumes are observed in drought years, 40 %–50 % at the peak month of the burning season (September) and 94 % over tropical forest and savanna regions, with respect to the total number of smoke plume observations. At the time of the MISR observations (10:00–11:00 LT), the highest plumes are detected over grassland fires (with an averaged maximum plume height of ∼1100 m) and the lowest plumes occur over tropical forest fires (∼800 m). A similar pattern is found later in the day (14:00–15:00 LT) with CALIOP, although at higher altitudes (2300 m grassland vs. 2000 m tropical forest), as CALIOP typically detects smoke at higher altitudes due to its later overpass time, associated with a deeper planetary boundary layer, possibly more energetic fires, and greater sensitivity to thin aerosol layers. On average, 3 %–20 % of the fires inject smoke into the free troposphere; this percentage tends to increase toward the end of the burning season (November: 15 %–40 %). We find a well-defined seasonal cycle between MISR plume heights, MODIS fire radiative power and atmospheric stability across the main biomes of the Amazon, with higher smoke plumes, more intense fires and reduced atmospheric stability conditions toward the end of the burning season. Lower smoke plume heights are detected during drought (800 m) compared to non-drought (1100 m) conditions, in particular over tropical forest and savanna fires. Drought conditions favour understory fires over tropical forest, which tend to produce smouldering combustion and low smoke injection heights. Droughts also seem to favour deeper boundary layers and the percentage of smoke plumes that reach the free troposphere is lower during these dry conditions. Consistent with previous studies, the MISR mid-visible aerosol optical depth demonstrates that smoke makes a significant contribution to the total aerosol loading over the Amazon, which in combination with lower injection heights in drought periods has important implications for air quality. This work highlights the importance of biome type, fire properties and atmospheric and drought conditions for plume dynamics and smoke loading. In addition, our study demonstrates the value of combining observations of MISR and CALIOP constraints on the vertical distribution of smoke from biomass burning over the Amazon.

scholarly journals Wildfire Smoke Particle Properties and Evolution, From Space-Based Multi-Angle Imaging II: The Williams Flats Fire during the FIREX-AQ Campaign

2020 ◽  
Vol 12 (22) ◽  
pp. 3823
Author(s):  
Katherine T. Junghenn Noyes ◽  
Ralph A. Kahn ◽  
James A. Limbacher ◽  
Zhanqing Li ◽  
Marta A. Fenn ◽  
...  
Keyword(s):  
Particle Size ◽  
Biomass Burning ◽  
In Situ Measurements ◽  
Statistical Characterization ◽  
Smoke Particle ◽  
Particle Properties ◽  
In Situ Data ◽  
Particle Property ◽  
Aircraft Data

Although the characteristics of biomass burning events and the ambient ecosystem determine emitted smoke composition, the conditions that modulate the partitioning of black carbon (BC) and brown carbon (BrC) formation are not well understood, nor are the spatial or temporal frequency of factors driving smoke particle evolution, such as hydration, coagulation, and oxidation, all of which impact smoke radiative forcing. In situ data from surface observation sites and aircraft field campaigns offer deep insight into the optical, chemical, and microphysical traits of biomass burning (BB) smoke aerosols, such as single scattering albedo (SSA) and size distribution, but cannot by themselves provide robust statistical characterization of both emitted and evolved particles. Data from the NASA Earth Observing System’s Multi-Angle Imaging SpectroRadiometer (MISR) instrument can provide at least a partial picture of BB particle properties and their evolution downwind, once properly validated. Here we use in situ data from the joint NOAA/NASA 2019 Fire Influence on Regional to Global Environments Experiment-Air Quality (FIREX-AQ) field campaign to assess the strengths and limitations of MISR-derived constraints on particle size, shape, light-absorption, and its spectral slope, as well as plume height and associated wind vectors. Based on the satellite observations, we also offer inferences about aging mechanisms effecting downwind particle evolution, such as gravitational settling, oxidation, secondary particle formation, and the combination of particle aggregation and condensational growth. This work builds upon our previous study, adding confidence to our interpretation of the remote-sensing data based on an expanded suite of in situ measurements for validation. The satellite and in situ measurements offer similar characterizations of particle property evolution as a function of smoke age for the 06 August Williams Flats Fire, and most of the key differences in particle size and absorption can be attributed to differences in sampling and changes in the plume geometry between sampling times. Whereas the aircraft data provide validation for the MISR retrievals, the satellite data offer a spatially continuous mapping of particle properties over the plume, which helps identify trends in particle property downwind evolution that are ambiguous in the sparsely sampled aircraft transects. The MISR data record is more than two decades long, offering future opportunities to study regional wildfire plume behavior statistically, where aircraft data are limited or entirely lacking.

scholarly journals Consistent regional fluxes of CH<sub>4</sub> and CO<sub>2</sub> inferred from GOSAT proxy XCH<sub>4</sub> : XCO<sub>2</sub> retrievals, 2010–2014

2017 ◽  
Vol 17 (7) ◽  
pp. 4781-4797 ◽  
Author(s):  
Liang Feng ◽  
Paul I. Palmer ◽  
Hartmut Bösch ◽  
Robert J. Parker ◽  
Alex J. Webb ◽  
...  
Keyword(s):  
South America ◽  
Large Scale ◽  
A Priori ◽  
Co2 Fluxes ◽  
A Posteriori ◽  
Data Products ◽  
The Tropics ◽  
Regional Fluxes ◽  
Tropical South America

Abstract. We use the GEOS-Chem global 3-D model of atmospheric chemistry and transport and an ensemble Kalman filter to simultaneously infer regional fluxes of methane (CH4) and carbon dioxide (CO2) directly from GOSAT retrievals of XCH4 : XCO2, using sparse ground-based CH4 and CO2 mole fraction data to anchor the ratio. This work builds on the previously reported theory that takes into account that (1) these ratios are less prone to systematic error than either the full-physics data products or the proxy CH4 data products; and (2) the resulting CH4 and CO2 fluxes are self-consistent. We show that a posteriori fluxes inferred from the GOSAT data generally outperform the fluxes inferred only from in situ data, as expected. GOSAT CH4 and CO2 fluxes are consistent with global growth rates for CO2 and CH4 reported by NOAA and have a range of independent data including new profile measurements (0–7 km) over the Amazon Basin that were collected specifically to help validate GOSAT over this geographical region. We find that large-scale multi-year annual a posteriori CO2 fluxes inferred from GOSAT data are similar to those inferred from the in situ surface data but with smaller uncertainties, particularly over the tropics. GOSAT data are consistent with smaller peak-to-peak seasonal amplitudes of CO2 than either the a priori or in situ inversion, particularly over the tropics and the southern extratropics. Over the northern extratropics, GOSAT data show larger uptake than the a priori but less than the in situ inversion, resulting in small net emissions over the year. We also find evidence that the carbon balance of tropical South America was perturbed following the droughts of 2010 and 2012 with net annual fluxes not returning to an approximate annual balance until 2013. In contrast, GOSAT data significantly changed the a priori spatial distribution of CH4 emission with a 40 % increase over tropical South America and tropical Asia and a smaller decrease over Eurasia and temperate South America. We find no evidence from GOSAT that tropical South American CH4 fluxes were dramatically affected by the two large-scale Amazon droughts. However, we find that GOSAT data are consistent with double seasonal peaks in Amazonian fluxes that are reproduced over the 5 years we studied: a small peak from January to April and a larger peak from June to October, which are likely due to superimposed emissions from different geographical regions.

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