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

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.

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.


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.


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.


2010 ◽  
Vol 10 (1) ◽  
pp. 977-1004
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 measurements of aerosol optical depth from the MODIS instruments onboard NASA's Terra and Aqua satellites, combined with the atmospheric chemical transport model MOZART. The model allows for an estimate of double counting of enhanced levels of aerosol optical depth in consecutive satellite overpasses. Using this method we infer an estimated total emission of 10±3 Tg of carbon monoxide from the Canberra fires of 2003. Emissions estimates for several other trace gases are also given. 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. The new method for estimating emissions from large vegetation fires described in this paper has some significant uncertainties, but these are mainly quantifiable and 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.


2014 ◽  
Vol 14 (23) ◽  
pp. 32177-32231 ◽  
Author(s):  
V. Buchard ◽  
A. M. da Silva ◽  
P. R. Colarco ◽  
A. Darmenov ◽  
C. A. Randles ◽  
...  

Abstract. A radiative transfer interface has been developed to simulate the UV Aerosol Index (AI) from the NASA Goddard Earth Observing System version 5 (GEOS-5) aerosol assimilated fields. The purpose of this work is to use the AI and Aerosol Absorption Optical Depth (AAOD) derived from the Ozone Monitoring Instrument (OMI) measurements as independent validation for the Modern Era Retrospective analysis for Research and Applications Aerosol Reanalysis (MERRAero). MERRAero is based on a version of the GEOS-5 model that is radiatively coupled to the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) aerosol module and includes assimilation of Aerosol Optical Depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor. Since AI is dependent on aerosol concentration, optical properties and altitude of the aerosol layer, we make use of complementary observations to fully diagnose the model, including AOD from the Multi-angle Imaging SpectroRadiometer (MISR), aerosol retrievals from the Aerosol Robotic Network (AERONET) and attenuated backscatter coefficients from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission to ascertain potential misplacement of plume height by the model. By sampling dust, biomass burning and pollution events in 2007 we have compared model produced AI and AAOD with the corresponding OMI products, identifying regions where the model representation of absorbing aerosols was deficient. As a result of this study over the Saharan dust region, we have obtained a new set of dust aerosol optical properties that retains consistency with the MODIS AOD data that were assimilated, while resulting in better agreement with aerosol absorption measurements from OMI. The analysis conducted over the South African and South American biomass burning regions indicates that revising the spectrally-dependent aerosol absorption properties in the near-UV region improves the modeled-observed AI comparisons. Finally, during a period where the Asian region was mainly dominated by anthropogenic aerosols, we have performed a qualitative analysis in which the specification of anthropogenic emissions in GEOS-5 is adjusted to provide insight into discrepancies observed in AI comparisons.


2010 ◽  
Vol 10 (24) ◽  
pp. 12273-12283 ◽  
Author(s):  
J. Kar ◽  
M. N. Deeter ◽  
J. Fishman ◽  
Z. Liu ◽  
A. Omar ◽  
...  

Abstract. A large wintertime increase in pollutants has been observed over the eastern parts of the Indo Gangetic Plains. We use improved version 4 carbon monoxide (CO) retrievals from the Measurements of Pollution in the Troposphere (MOPITT) along with latest version 3 aerosol data from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) lidar instrument and the tropospheric ozone residual products to characterize this pollution pool. The feature is seen primarily in the lower troposphere from about November to February with strong concomitant increases in CO and aerosol optical depth (AOD). The signature of the feature is also observed in tropospheric ozone column data. The height resolved aerosol data from CALIPSO confirm the trapping of the pollution pool at the lowest altitudes. The observations indicate that MOPITT can capture this low altitude phenomenon even in winter conditions as indicated by the averaging kernels.


Tellus B ◽  
2000 ◽  
Vol 52 (2) ◽  
pp. 594-619
Author(s):  
John M. Livingstone ◽  
Vladimir N. Kapustin ◽  
Beat Schmid ◽  
Philip B. Russel ◽  
Patricia K. Quinn ◽  
...  

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