scholarly journals Modelling the optical properties of fresh biomass burning aerosol produced in a smoke chamber: results from the EFEU campaign

2007 ◽  
Vol 7 (4) ◽  
pp. 12657-12686 ◽  
Author(s):  
K. Hungershöfer ◽  
K. Zeromskiene ◽  
Y. Iinuma ◽  
G. Helas ◽  
J. Trentmann ◽  
...  

Abstract. A better characterisation of the optical properties of biomass burning aerosol as a function of the burning conditions is required in order to quantify their effects on climate and atmospheric chemistry. Controlled laboratory combustion experiments with different fuel types were carried out at the combustion facility of the Max Planck Institute for Chemistry (Mainz, Germany) as part of the 'Impact of Vegetation Fires on the Composition and Circulation of the Atmosphere' (EFEU) project. Using the measured size distributions as well as mass scattering and absorption efficiencies, Mie calculations provided mean effective refractive indices of 1.60−0.010i and 1.56−0.010i (λ=0.55 μm) for smoke particles emitted from the combustion of savanna grass and an African hardwood (musasa), respectively. The relatively low imaginary parts suggest that the light-absorbing carbon of the investigated fresh biomass burning aerosol is only partly graphitized, resulting in strongly scattering and less absorbing particles. While the observed variability in mass scattering efficiencies was consistent with changes in particle size, the changes in the mass absorption efficiency can only be explained, if the chemical composition of the particles varies with combustion conditions.

2008 ◽  
Vol 8 (13) ◽  
pp. 3427-3439 ◽  
Author(s):  
K. Hungershoefer ◽  
K. Zeromskiene ◽  
Y. Iinuma ◽  
G. Helas ◽  
J. Trentmann ◽  
...  

Abstract. A better characterisation of the optical properties of biomass burning aerosol as a function of the burning conditions is required in order to quantify their effects on climate and atmospheric chemistry. Controlled laboratory combustion experiments with different fuel types were carried out at the combustion facility of the Max Planck Institute for Chemistry (Mainz, Germany) as part of the "Impact of Vegetation Fires on the Composition and Circulation of the Atmosphere" (EFEU) project. The combustion conditions were monitored with concomitant CO2 and CO measurements. The mass scattering efficiencies of 8.9±0.2 m2 g−1 and 9.3±0.3 m2 g−1 obtained for aerosol particles from the combustion of savanna grass and an African hardwood (musasa), respectively, are larger than typically reported mainly due to differences in particle size distribution. The photoacoustically measured mass absorption efficiencies of 0.51±0.02 m2 g−1 and 0.50±0.02 m2 g−1 were at the lower end of the literature values. Using the measured size distributions as well as the mass scattering and absorption efficiencies, Mie calculations provided effective refractive indices of 1.60−0.010i (savanna grass) and 1.56−0.010i (musasa) (λ=0.55 μm). The apparent discrepancy between the low imaginary part of the refractive index and the high apparent elemental carbon (ECa) fractions (8 to 15%) obtained from the thermographic analysis of impactor samples can be explained by a positive bias in the elemental carbon data due to the presence of high molecular weight organic substances. Potential artefacts in optical properties due to instrument bias, non-natural burning conditions and unrealistic dilution history of the laboratory smoke cannot be ruled out and are also discussed in this study.


2019 ◽  
Vol 19 (9) ◽  
pp. 6561-6577 ◽  
Author(s):  
Emily Ramnarine ◽  
John K. Kodros ◽  
Anna L. Hodshire ◽  
Chantelle R. Lonsdale ◽  
Matthew J. Alvarado ◽  
...  

Abstract. Biomass burning is a significant global source of aerosol number and mass. In fresh biomass burning plumes, aerosol coagulation reduces aerosol number and increases the median size of aerosol size distributions, impacting aerosol radiative effects. Near-source biomass burning aerosol coagulation occurs at spatial scales much smaller than the grid boxes of global and many regional models. To date, these models have ignored sub-grid coagulation and instantly mixed fresh biomass burning emissions into coarse grid boxes. A previous study found that the rate of particle growth by coagulation within an individual smoke plume can be approximated using the aerosol mass emissions rate, initial size distribution median diameter and modal width, plume mixing depth, and wind speed. In this paper, we use this parameterization of sub-grid coagulation in the GEOS-Chem–TOMAS (TwO-Moment Aerosol Sectional) global aerosol microphysics model to quantify the impacts on global aerosol size distributions, the direct radiative effect, and the cloud-albedo aerosol indirect effect. We find that inclusion of biomass burning sub-grid coagulation reduces the biomass burning impact on the number concentration of particles larger than 80 nm (a proxy for CCN-sized particles) by 37 % globally. This cloud condensation nuclei (CCN) reduction causes our estimated global biomass burning cloud-albedo aerosol indirect effect to decrease from −76 to −43 mW m−2. Further, as sub-grid coagulation moves mass to sizes with more efficient scattering, including it increases our estimated biomass burning all-sky direct effect from −224 to −231 mW m−2, with assumed external mixing of black carbon and from −188 to −197 mW m−2 and with assumed internal mixing of black carbon with core-shell morphology. However, due to differences in fire and meteorological conditions across regions, the impact of sub-grid coagulation is not globally uniform. We also test the sensitivity of the impact of sub-grid coagulation to two different biomass burning emission inventories to various assumptions about the fresh biomass burning aerosol size distribution and to two different timescales of sub-grid coagulation. The impacts of sub-grid coagulation are qualitatively the same regardless of these assumptions.


2018 ◽  
Author(s):  
Emily Ramnarine ◽  
John K. Kodros ◽  
Anna L. Hodshire ◽  
Chantelle R. Lonsdale ◽  
Matthew J. Alvarado ◽  
...  

Abstract. Biomass burning is a significant global source of aerosol number and mass. In fresh biomass burning plumes, aerosol coagulation reduces aerosol number and increases the median size of aerosol size distributions, impacting aerosol radiative effects. Near-source biomass burning aerosol coagulation occurs at spatial scales much smaller than the grid boxes of global and many regional models. To date, these models ignore sub-grid coagulation and instantly mix fresh biomass burning emissions into coarse grid boxes. A previous study found that the rate of particle growth by coagulation within an individual smoke plume can be approximated using the aerosol mass emissions rate, initial size distribution median diameter and modal width, plume mixing depth, and wind speed. In this paper, we use this parameterization of sub-grid coagulation in the GEOS-Chem-TOMAS global aerosol microphysics model to quantify the impacts on global aerosol size distributions, the direct radiative effect, and the cloud-albedo aerosol indirect effect. We find that inclusion of biomass burning sub-grid coagulation reduces the biomass burning impact on the number concentration of particles larger than 80 nm (a proxy for CCN-sized particles) by 37 % globally. This CCN reduction causes our estimated global biomass burning cloud-albedo aerosol indirect effect to decrease from −76 to −43 mW m−2. Further, as sub-grid coagulation moves mass to sizes with more efficient scattering, including it increases our estimated biomass burning all-sky direct effect from −224 to −231 mW m−2 with assumed external mixing and from −188 to −197 mW m−2 with assumed internal mixing with core-shell morphology. However, due to differences in fire and meteorological conditions across regions, the impact of sub-grid coagulation is not globally uniform. We also test the sensitivity of the impact of sub-grid coagulation to two different biomass burning emission inventories, to various assumptions about the fresh biomass burning aerosol size distribution, and to two different timescales of sub-grid coagulation. The impacts of sub-grid coagulation are qualitatively the same regardless of these assumptions.


2010 ◽  
Vol 10 (12) ◽  
pp. 5391-5408 ◽  
Author(s):  
J. Jung ◽  
Y. J. Kim ◽  
K. Y. Lee ◽  
M. G. -Cayetano ◽  
T. Batmunkh ◽  
...  

Abstract. As a part of the IGAC (International Global Atmospheric Chemistry) Mega-cities program, aerosol physical and optical properties were continuously measured from March 2007 to March 2008 at an urban site (37.57° N, 126.94° E) in Seoul, Korea. Spectral optical properties of long-range transported Asian dust and pollution aerosols have been investigated based on the year long measurement data. Optically measured black carbon/thermally measured elemental carbon (BC/EC) ratio showed clear monthly variation with high values in summer and low values in winter mainly due to the enhancement of light attenuation by the internal mixing of EC. Novel approach has been suggested to retrieve the spectral light absorption coefficient (babs) from Aethalometer raw data by using BC/EC ratio. Mass absorption efficiency, σabs (=babs/EC) at 550 nm was determined to be 9.0±1.3, 8.9±1.5, 9.5±2.0, and 10.3±1.7 m2 g−1 in spring, summer, fall, and winter, respectively with an annual mean of 9.4±1.8 m2 g−1. Threshold values to classify severe haze events were suggested in this study. Increasing trend of aerosol single scattering albedo (SSA) with wavelength was observed during Asian dust events while little spectral dependence of SSA was observed during long-range transport pollution (LTP) events. Satellite aerosol optical thickness (AOT) and Hysplit air mass backward trajectory analyses as well as chemical analysis were performed to characterize the dependence of spectral optical properties on aerosol type. Results from this study can provide useful information for studies on regional air quality and aerosol's effects on climate change.


2019 ◽  
Vol 19 (14) ◽  
pp. 9181-9208 ◽  
Author(s):  
Kristina Pistone ◽  
Jens Redemann ◽  
Sarah Doherty ◽  
Paquita Zuidema ◽  
Sharon Burton ◽  
...  

Abstract. The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol–cloud–radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here, we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single-scattering albedo. Most but not all of the biomass burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60 %. We present the single-scattering albedo (SSA), absorbing and total aerosol optical depth (AAOD and AOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, and EAE, respectively) for specific case studies looking at near-coincident and near-colocated measurements from multiple instruments, and SSAs for the broader campaign average over the month-long deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD400>0.4). The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 nm (SSA500) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the interquartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences.


2019 ◽  
Vol 19 (23) ◽  
pp. 14805-14824
Author(s):  
Aurélien Chauvigné ◽  
Diego Aliaga ◽  
Karine Sellegri ◽  
Nadège Montoux ◽  
Radovan Krejci ◽  
...  

Abstract. This study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240 m a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz–El Alto, located approximately 20 km away and 1.5 km below the sampling site. The extended multi-year record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96 Mm−1 respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68 Mm−1 respectively) and higher values during the dry season (0.80, 11.23, and 14.51 Mm−1 respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz–El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28 % to 80 % increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere.


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