Abstract. Black carbon (BC) emissions from open biomass burning (BB) are known to have a considerable impact on the radiative budget of the atmosphere at both global and regional scales; however, these emissions are poorly constrained in models by atmospheric observations, especially in remote regions. Here, we investigate the feasibility of constraining BC emissions from BB using satellite observations of the aerosol absorption optical depth (AAOD) and the aerosol extinction optical depth (AOD) retrieved from OMI (Ozone Monitoring Instrument) and MODIS (Moderate Resolution Imaging Spectroradiometer) measurements, respectively. We consider the case of Siberian BB BC emissions, which have the strong potential to impact the Arctic climate system. Using aerosol remote sensing data collected at Siberian sites of the AErosol RObotic NETwork (AERONET) along with the results of the fourth Fire Lab at Missoula Experiment (FLAME-4), we establish an empirical parameterization relating the ratio of the elemental carbon (EC) and organic carbon (OC) contents in BB aerosol to the ratio of AAOD and AOD at the wavelengths of the satellite observations. Applying this parameterization to the BC and OC column amounts simulated using the CHIMERE chemistry transport model, we optimize the parameters of the BB emission model based on MODIS measurements of the fire radiative power (FRP); we then obtain top-down optimized estimates of the total monthly BB BC amounts emitted from intense Siberian fires that occurred from May to September 2012. The top-down estimates are compared to the corresponding values obtained using the Global Fire Emissions Database (GFED4) and the Fire Emission Inventory–northern Eurasia (FEI-NE). Our simulations using the optimized BB aerosol emissions are verified against AAOD and AOD data that were withheld from the estimation procedure. The simulations are further evaluated against in situ EC and OC measurements at the Zotino Tall Tower Observatory (ZOTTO) and also against aircraft aerosol measurement data collected in the framework of the Airborne Extensive Regional Observations in SIBeria (YAK-AEROSIB) experiments. We conclude that our BC and OC emission estimates, considered with their confidence intervals, are consistent with the ensemble of the measurement data analyzed in this study. Siberian fires are found to emit 0.41±0.14 Tg of BC over the whole 5-month period considered; this estimate is a factor of 2 larger and a factor of 1.5 smaller than the corresponding estimates based on the GFED4 (0.20 Tg) and FEI-NE (0.61 Tg) data, respectively. Our estimates of monthly BC emissions are also found to be larger than the BC amounts calculated using the GFED4 data and smaller than those calculated using the FEI-NE data for any of the 5 months. Particularly large positive differences of our monthly BC emission estimates with respect to the GFED4 data are found in May and September. This finding indicates that the GFED4 database is likely to strongly underestimate BC emissions from agricultural burns and grass fires in Siberia. All of these differences have important implications for climate change in the Arctic, as it is found that about a quarter of the huge BB BC mass emitted in Siberia during the fire season of 2012 was transported across the polar circle into the Arctic. Overall, the results of our analysis indicate that a combination of the available satellite observations of AAOD and AOD can provide the necessary constraints on BB BC emissions.
Reliable assessment of the impact of Siberian boreal forest wildfires on the environment and climate necessitates an improved understanding of microphysical and chemical properties of emitted aerosols. Smoldering, flaming and mixed fires of typical Siberian biomass (pine and debris) were simulated during a small-scale study in a Large Aerosol Chamber (LAC). Individual particle analysis of PM 10 and PM 2.5 smoke morphology and elemental composition revealed a strong dependence on combustion temperature, i.e., a dominant abundance of soot agglomerates versus roughly spherical organic particles in the flaming and smoldering phase, respectively. Cluster analysis of smoke microstructure was used to apportion the emitted particles into major characteristic groups: Soot and Organic, which accounted for around 90% and 60% of total particle numbers emitted from the flaming and smoldering fires, respectively. Carbon fractions and inorganic ion analysis supported the identification of particle types representative of combustion phase and biomass type. Elemental carbon (EC) particles from flaming fires comprised approximately 25% of Group Soot, in good agreement with a high EC fraction in total carbon of around 65% and low organic carbon (OC)/EC ratio near 0.5. Smoldering fires of pine and debris produced exclusively organic particles with high OC/EC ratios of 194 and 34, respectively. Small quantities of elemental constituents in biomass were vaporized during combustion and produced internally/externally mixed fly ash in Group Ca-, Si-, and Fe-rich of significantly less abundance. Ca, Cl, S, and Mg were more frequently distributed elements in pine than debris smoke. Sulfates and nitrates produced from gas-to-particle reactions formed Group S-and N-rich. During time evolution of smoke volatile inorganic compounds were condensed as potassium chlorides and sulfates into a newly formed Group K,Cl-rich. Quantification of Siberian biomass smoke microstructure by chemical micromarkers enables aerosols to be classified with respect to a source type assigned to Siberian wildfires.
Abstract. An empirical model of the vertical profiles of aerosol optical characteristics is described. This model was developed based on data acquired from multi-year airborne sensing of optical and microphysical characteristics of the tropospheric aerosol over West Siberia. The main initial characteristics for the creation of the model were measurement data of the vertical profiles of the aerosol angular scattering coefficients in the visible wavelength range, particle size distribution functions and mass concentrations of black carbon (BC). The proposed model allows us to retrieve the aerosol optical and radiative characteristics in the visible and near-IR wavelength range, using the season, air mass type and time of day as input parameters. The columnar single scattering albedo and asymmetry factor of the aerosol scattering phase function, calculated using the average vertical profiles, are in good agreement with data from the AERONET station located in Tomsk.For solar radiative flux calculations, this empirical model has been tested for typical summer conditions. The available experimental database obtained for the regional features of West Siberia and the model developed on this basis are shown to be sufficient for performing these calculations.
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