scholarly journals Supplementary material to "Probing into the aging dynamics of biomass burning aerosol by using satellite measurements of aerosol optical depth and carbon monoxide"

Author(s):  
Igor B. Konovalov ◽  
Matthias Beekmann ◽  
Evgeny V. Berezin ◽  
Paola Formenti ◽  
Meinrat O. Andreae
2016 ◽  
Author(s):  
Igor B. Konovalov ◽  
Matthias Beekmann ◽  
Evgeny V. Berezin ◽  
Paola Formenti ◽  
Meinrat O. Andreae

Abstract. Carbonaceous aerosol released into the atmosphere from open biomass burning (BB) is known to undergo considerable chemical and physical transformations (aging). However, there exists substantial controversy about the nature and observable effects of these transformations. A shortage of consistent observational evidence on BB aerosol aging processes in different environmental conditions and at various temporal scales hinders developing their adequate representations in chemistry transport models (CTMs). In this study, we obtain insights into the BB aerosol dynamics by using available satellite measurements of aerosol optical depth (AOD) and carbon monoxide (CO). The basic concept of our method is to consider AOD as a function of the BB aerosol "photochemical age" (that is, the time period characterizing the exposure of BB aerosol emissions to atmospheric oxidation reactions) predicted by means of model tracers. We evaluate the AOD enhancement ratio (ER) defined as the ratio of optical depth of actual BB aerosol with respect to that of a modeled aerosol tracer that is assumed to originate from the same fires as the real BB aerosol but is not affected by any aging processes. To limit possible effects of model transport errors, the AOD measurements are normalized to CO column amounts that are also retrieved from satellite measurements. The method is applied to the analysis of the meso- and synoptic-scale evolution of aerosol in smoke plumes from major wildfires that occurred in Siberia in summer 2012. AOD and CO retrievals from, respectively, MODIS and IASI measurements are used in combination with simulations performed with the CHIMERE CTM. The analysis indicates that aging processes strongly affected the evolution of BB aerosol in the situation considered, especially in dense plumes (with PM2.5 concentration exceeding 100 μg m−3). For such plumes, the ER is found to increase almost twofold on the scale of ~ 10 hours of the daytime evolution of aerosol (after a few first hours of the evolution that are not resolved in our analysis). The robustness of this finding is corroborated by sensitivity tests and Monte Carlo experiments. Furthermore, a simulation using the volatility basis set framework suggests that a large part of the increase in the ER can be explained by atmospheric processing of semi-volatile organic compounds. Our results are consistent with findings of a number of earlier studies reporting considerable underestimation of AOD by CTMs in which BB aerosol aging processes have either been disregarded or simulated in a highly simplified way. In general, this study demonstrates the feasibility of using satellite measurements of AOD in biomass burning plumes in combination with aerosol tracer simulations for the investigation of BB aerosol evolution and validation of BB aerosol aging schemes in atmospheric models.


2017 ◽  
Vol 17 (7) ◽  
pp. 4513-4537 ◽  
Author(s):  
Igor B. Konovalov ◽  
Matthias Beekmann ◽  
Evgeny V. Berezin ◽  
Paola Formenti ◽  
Meinrat O. Andreae

Abstract. Carbonaceous aerosol released into the atmosphere from open biomass burning (BB) is known to undergo considerable chemical and physical transformations (aging). However, there is substantial controversy about the nature and observable effects of these transformations. A shortage of consistent observational evidence on BB aerosol aging processes under different environmental conditions and at various temporal scales hinders development of their adequate representations in chemistry transport models (CTMs). In this study, we obtain insights into the BB aerosol dynamics by using available satellite measurements of aerosol optical depth (AOD) and carbon monoxide (CO). The basic concept of our method is to consider AOD as a function of the BB aerosol photochemical age (that is, the time period characterizing the exposure of BB aerosol emissions to atmospheric oxidation reactions) predicted by means of model tracers. We evaluate the AOD enhancement ratio (ER) defined as the ratio of optical depth of actual BB aerosol with respect to that of a modeled aerosol tracer that is assumed to originate from the same fires as the real BB aerosol but that is not affected by any aging processes. To limit possible effects of model transport errors, the AOD measurements are normalized to CO column amounts that are also retrieved from satellite measurements. The method is applied to the analysis of the meso- and synoptic-scale evolution of aerosol in smoke plumes from major wildfires that occurred in Siberia in summer 2012. AOD and CO retrievals from MODIS and IASI measurements, respectively, are used in combination with simulations performed with the CHIMERE CTM. The analysis indicates that aging processes strongly affected the evolution of BB aerosol in the situation considered, especially in dense plumes (with spatial average PM2. 5 concentration exceeding 100 µg m−3). For such plumes, the ER is found to increase almost 2-fold on the scale of ∼ 10 h of daytime aerosol evolution (after a few first hours of the evolution that are not resolved in our analysis). The robustness of this finding is corroborated by sensitivity tests and Monte Carlo experiments. Furthermore, a simulation using the volatility basis set framework suggests that a large part of the increase in the ER can be explained by atmospheric processing of semi-volatile organic compounds. Our results are consistent with findings of a number of earlier studies reporting considerable underestimation of AOD by CTMs in which BB aerosol aging processes have either been disregarded or simulated in a highly simplified way. In general, this study demonstrates the feasibility of using satellite measurements of AOD in biomass burning plumes in combination with aerosol tracer simulations for the investigation of BB aerosol evolution and validation of BB aerosol aging schemes in atmospheric models.


2010 ◽  
Vol 10 (12) ◽  
pp. 5739-5748 ◽  
Author(s):  
C. Paton-Walsh ◽  
L. K. Emmons ◽  
S. R. Wilson

Abstract. In this paper we describe a new method for estimating trace gas emissions from large vegetation fires using satellite measurements of aerosol optical depth (AOD) at 550 nm, combined with an atmospheric chemical transport model. The method uses a threshold value to screen out normal levels of AOD that may be caused by raised dust, sea salt aerosols or diffuse smoke transported from distant fires. Using this method we infer an estimated total emission of 15±5 Tg of carbon monoxide, 0.05±0.02 Tg of hydrogen cyanide, 0.11±0.03 Tg of ammonia, 0.25±0.07 Tg of formaldehyde, 0.03±0.01 of acetylene, 0.10±0.03 Tg of ethylene, 0.03±0.01 Tg of ethane, 0.21±0.06 Tg of formic acid and 0.28±0.09 Tg of methanol released to the atmosphere from the Canberra fires of 2003. An assessment of the uncertainties in the new method is made and we show that our estimate agrees (within expected uncertainties) with estimates made using current conventional methods of multiplying together factors for the area burned, fuel load, the combustion efficiency and the emission factor for carbon monoxide. A simpler estimate derived directly from the satellite AOD measurements is also shown to be in agreement with conventional estimates, suggesting that the method may, under certain meteorological conditions, be applied without the complication of using a chemical transport model. The new method is suitable for estimating emissions from distinct large fire episodes and although it has some significant uncertainties, these are largely independent of the uncertainties inherent in conventional techniques. Thus we conclude that the new method is a useful additional tool for characterising emissions from vegetation fires.


2019 ◽  
Author(s):  
Samuel E. LeBlanc ◽  
Jens Redemann ◽  
Connor Flynn ◽  
Kristina Pistone ◽  
Meloë Kacenelenbogen ◽  
...  

Abstract. The South-East Atlantic (SEA) is host to a climatologically significant biomass burning aerosol layer overlying marine stratocumulus. We present directly measured Above Cloud Aerosol Optical Depth (ACAOD) from the recent ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) airborne field campaign during August and September 2016. In our analysis, we use data from the Spectrometers for Sky-Scanning Sun-Tracking Atmospheric Research (4STAR) instrument and found an average ACAOD of 0.32 at 501 nm, with an average Ångström exponent (AE) of 1.71. The AE is much lower at 1.25 for the full column (including below cloud level aerosol), indicating the presence of large aerosol particles, likely marine aerosol, embedded within the vertical column. ACAOD is observed to be highest near coast at about 12° S, whereas its variability is largest at the southern edge of the average aerosol plume, as indicated by 12 years of MODIS observations. In comparison to MODIS derived ACAOD and long term fine-mode plume-average AOD, the directly-measured ACAOD from 4STAR is slightly lower than the ACAOD product from MODIS. The peak ACAOD expected from long term retrievals is measured to be closer to coast in 2016 at about 1.5°–4° W. By spatially binning the sampled AOD, we obtain a mean ACAOD of 0.37 for the SEA region. Vertical profiles of AOD showcase the variability of the altitude of the aerosol plume and its separation from cloud top. We measured larger AOD at high altitude near coast than farther from coast, while generally observing a larger vertical gap further from coast. Changes of AOD with altitude are correlated with a gas tracer of the biomass burning aerosol plume. Vertical extent of gaps between aerosol and cloud show a large distribution of extent, dominated by near zero gap. The gap distribution with longitude is observed to be largest at about 7° W, farther from coast than expected.


2020 ◽  
Vol 20 (3) ◽  
pp. 1565-1590 ◽  
Author(s):  
Samuel E. LeBlanc ◽  
Jens Redemann ◽  
Connor Flynn ◽  
Kristina Pistone ◽  
Meloë Kacenelenbogen ◽  
...  

Abstract. The southeast Atlantic (SEA) region is host to a climatologically significant biomass burning aerosol layer overlying marine stratocumulus. We present the first results of the directly measured above-cloud aerosol optical depth (ACAOD) from the recent ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) airborne field campaign during August and September 2016. In our analysis, we use data from the Spectrometers for Sky-Scanning Sun-Tracking Atmospheric Research (4STAR) instrument and found an average ACAOD of 0.32 at 501 nm (range of 0.02 to 1.04), with an average Ångström exponent (AE) above clouds of 1.71. The AE is much lower at 1.25 for the full column (including below-cloud-level aerosol, with an average of 0.36 at 501 nm and a range of 0.02 to 0.74), indicating the presence of large aerosol particles, likely marine aerosol, in the lower atmospheric column. The ACAOD is observed from 4STAR to be highest near the coast at about 12∘ S, whereas its variability is largest at the southern edge of the average aerosol plume, as indicated by 12 years of MODIS observations. In comparison to MODIS-derived ACAOD and long-term fine-mode plume-average AOD along a diagonal routine track extending out from the coast of Namibia, the directly measured ACAOD from 4STAR is slightly lower than the ACAOD product from MODIS. The peak ACAOD expected from MODIS AOD retrievals averaged over a long term along the routine diagonal flight track (peak of 0.5) was measured to be closer to coast in 2016 at about 1.5–4∘ E, with 4STAR ACAOD averages showing a peak of 0.42. When considering the full observation set over the SEA, by spatially binning each sampled AOD, we obtain a geographically representative mean ACAOD of 0.37. Vertical profiles of AOD showcase the variability in the altitude of the aerosol plume and its separation from the cloud top. We measured larger AOD at a high altitude near the coast than farther from the coast, while generally observing a larger vertical gap farther from the coast. Changes in AOD with altitude are correlated with carbon monoxide, a gas tracer of the biomass burning aerosol plume. Vertical extent of gaps between aerosol and cloud show a wide distribution, with a near-zero gap being most frequent. The gap distribution with longitude is observed to be largest at about 7∘ E, farther from coast than expected from previous studies.


2021 ◽  
Vol 13 (11) ◽  
pp. 2231
Author(s):  
Débora Souza Alvim ◽  
Júlio Barboza Chiquetto ◽  
Monica Tais Siqueira D’Amelio ◽  
Bushra Khalid ◽  
Dirceu Luis Herdies ◽  
...  

The scope of this work was to evaluate simulated carbon monoxide (CO) and aerosol optical depth (AOD) from the CAM-chem model against observed satellite data and additionally explore the empirical relationship of CO, AOD and fire radiative power (FRP). The simulated seasonal global concentrations of CO and AOD were compared, respectively, with the Measurements of Pollution in the Troposphere (MOPITT) and the Moderate-Resolution Imaging Spectroradiometer (MODIS) satellite products for the period 2010–2014. The CAM-chem simulations were performed with two configurations: (A) tropospheric-only; and (B) tropospheric with stratospheric chemistry. Our results show that the spatial and seasonal distributions of CO and AOD were reasonably reproduced in both model configurations, except over central China, central Africa and equatorial regions of the Atlantic and Western Pacific, where CO was overestimated by 10–50 ppb. In configuration B, the positive CO bias was significantly reduced due to the inclusion of dry deposition, which was not present in the model configuration A. There was greater CO loss due to the chemical reactions, and shorter lifetime of the species with stratospheric chemistry. In summary, the model has difficulty in capturing the exact location of the maxima of the seasonal AOD distributions in both configurations. The AOD was overestimated by 0.1 to 0.25 over desert regions of Africa, the Middle East and Asia in both configurations, but the positive bias was even higher in the version with added stratospheric chemistry. By contrast, the AOD was underestimated over regions associated with anthropogenic activity, such as eastern China and northern India. Concerning the correlations between CO, AOD and FRP, high CO is found during March–April–May (MAM) in the Northern Hemisphere, mainly in China. In the Southern Hemisphere, high CO, AOD, and FRP values were found during August–September–October (ASO) due to fires, mostly in South America and South Africa. In South America, high AOD levels were observed over subtropical Brazil, Paraguay and Bolivia. Sparsely urbanized regions showed higher correlations between CO and FRP (0.7–0.9), particularly in tropical areas, such as the western Amazon region. There was a high correlation between CO and aerosols from biomass burning at the transition between the forest and savanna environments over eastern and central Africa. It was also possible to observe the transport of these pollutants from the African continent to the Brazilian coast. High correlations between CO and AOD were found over southeastern Asian countries, and correlations between FRP and AOD (0.5–0.8) were found over higher latitude regions such as Canada and Siberia as well as in tropical areas. Higher correlations between CO and FRP are observed in Savanna and Tropical forests (South America, Central America, Africa, Australia, and Southeast Asia) than FRP x AOD. In contrast, boreal forests in Russia, particularly in Siberia, show a higher FRP x AOD correlation than FRP x CO. In tropical forests, CO production is likely favored over aerosol, while in temperate forests, aerosol production is more than CO compared to tropical forests. On the east coast of the United States, the eastern border of the USA with Canada, eastern China, on the border between China, Russia, and Mongolia, and the border between North India and China, there is a high correlation of CO x AOD and a low correlation between FRP with both CO and AOD. Therefore, such emissions in these regions are not generated by forest fires but by industries and vehicular emissions since these are densely populated regions.


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