scholarly journals Physical and Optical Properties of Aged Biomass Burning Aerosol from Wildfires in Siberia and the Western US at the Mt. Bachelor Observatory

Author(s):  
James R. Laing ◽  
Dan A. Jaffe ◽  
Jonathan R. Hee

Abstract. The summer of 2015 was an extreme forest fire year in the Pacific North West. Our sample site at Mt. Bachelor Observatory (MBO, 2.7 km a.s.l.) in central Oregon observed biomass burning events more than 50 % of the time during August. In this paper we characterize the aerosol physical and optical properties of 19 aged biomass burning (BB) events during August 2015. Six of the nineteen events were influenced by Siberian fires originating near Lake Baikal. The remainder of the events resulted from wildfires in Northern California and Southwestern Oregon with transport times to MBO ranging from 4.5–35 hours. Fine particulate matter (PM1), carbon monoxide (CO), aerosol light scattering (σscat) and absorption (σabs), and aerosol number size distributions were measured throughout the campaign. We found that the Siberian events had significantly higher Δσabs/ΔCO enhancement ratio, higher mass absorption efficiency (MAE; Δσabs/ΔPM1), lower single scattering albedo (ω), and lower Absorption Ångström exponent (AAE) when compared with the regional events. We suspect the Siberian events observed represent a portion of the fire plume that has hotter flaming fire conditions that enabled strong pyro-convective lofting and long transport to MBO. These plumes would then have preferentially higher black carbon emissions and thus absorption enhancement. The lower AAE values in the Siberian events compared to regional events indicates a lack of brown carbon (BrC) production by the Siberian fires or a loss of BrC during transport. We found that mass scattering efficiencies (MSE) for the BB events to range from 2.50–4.76 m2 g−1. We measured aerosol size distributions with a scanning mobility particle sizer (SMPS). Number size distributions ranged from unimodal to bimodal and had geometric mean diameters ranging from 138–229 nm and geometric standard deviations ranging from 1.53–1.89. We found MSE’s for BB events to be positively correlated with the geometric mean of the aerosol size distributions (R2 = 0.73), which agrees with Mie Theory. We did not find any dependence on event size distribution to transport time or fire source location.

2016 ◽  
Vol 16 (23) ◽  
pp. 15185-15197 ◽  
Author(s):  
James R. Laing ◽  
Daniel A. Jaffe ◽  
Jonathan R. Hee

Abstract. The summer of 2015 was an extreme forest fire year in the Pacific Northwest. Our sample site at the Mt. Bachelor Observatory (MBO, 2.7 km a.s.l.) in central Oregon observed biomass burning (BB) events more than 50 % of the time during August. In this paper we characterize the aerosol physical and optical properties of 19 aged BB events during August 2015. Six of the 19 events were influenced by Siberian fires originating near Lake Baikal that were transported to MBO over 4–10 days. The remainder of the events resulted from wildfires in Northern California and Southwestern Oregon with transport times to MBO ranging from 3 to 35 h. Fine particulate matter (PM1), carbon monoxide (CO), aerosol light scattering coefficients (σscat), aerosol light absorption coefficients (σabs), and aerosol number size distributions were measured throughout the campaign. We found that the Siberian events had a significantly higher Δσabs∕ΔCO enhancement ratio, higher mass absorption efficiency (MAE; Δσabs∕ΔPM1), lower single scattering albedo (ω), and lower absorption Ångström exponent (AAE) when compared with the regional events. We suggest that the observed Siberian events represent that portion of the plume that has hotter flaming fire conditions and thus enabled strong pyroconvective lofting and long-range transport to MBO. The Siberian events observed at MBO therefore represent a selected portion of the original plume that would then have preferentially higher black carbon emissions and thus an enhancement in absorption. The lower AAE values in the Siberian events compared to regional events indicate a lack of brown carbon (BrC) production by the Siberian fires or a loss of BrC during transport. We found that mass scattering efficiencies (MSE) for the BB events ranged from 2.50 to 4.76 m2 g−1. We measured aerosol size distributions with a scanning mobility particle sizer (SMPS). Number size distributions ranged from unimodal to bimodal and had geometric mean diameters (Dpm) ranging from 138 to 229 nm and geometric standard deviations (σg) ranging from 1.53 to 1.89. We found MSEs for BB events to be positively correlated with the geometric mean of the aerosol size distributions (R2 = 0.73), which agrees with Mie theory. We did not find any dependence on event size distribution to transport time or fire source location.


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.


2020 ◽  
Author(s):  
Archita Rana ◽  
Supriya Dey ◽  
Sayantan Sarkar

<p>Black and brown carbon (BC and BrC) are potent climate forcing agents with pronounced effects on global climate and tropospheric chemistry. Given the large heterogeneities in BC emission inventories from India and the paucity of studies on BrC characteristics, field-based measurements of BC and BrC sources and optical properties are essential to understand their impacts on regional climate. To address this issue, we report the first ground-based measurements of BC and BrC from a rural location in the highly polluted eastern Indo-Gangetic Plain (IGP) during May-November 2018 encompassing the photochemistry-dominated summer (May-June) and regional biomass burning (BB)-dominated post-monsoon (October-November) periods. A 7-wavelength Aethalometer was used for time-resolved measurements of BC mass and was supplemented by UV-Vis and fluorescence measurements of time-integrated (24 h) aqueous and organic BrC fractions, and measurements of OC, EC, WSOC, and ionic species.<br>The daily averaged BC increased 4 times during the BB regime (12.3 ± 3.9 μg m<sup>-3</sup>) as compared to summer (4.2 ± 0.8 μg m<sup>-3</sup>), while aqueous and organic BrC fractions demonstrated light absorption (babs_365) enhancements of 3-5 times during BB. For aqueous BrC, the averaged AE of 5.9-6.2 and a prominent fluorescence peak at ~420 nm suggested the presence of humic-like substances (HULIS), potentially from secondary photochemical formation during summer and primary emission during BB periods. Fluorescence and UV-Vis spectra also indicated the presence of nitroaromatic compounds, presumably from OH oxidation in summer and nighttime NO3- oxidation in the presence of enhanced NOx and precursor emission during BB. The latter was supported by the strong association between water-soluble organic carbon (WSOC; a proxy for aqueous BrC) and aerosol NO<sub>3</sub><sup>-</sup> (r=0.70, p<0.05). During BB, the fraction of water-insoluble (i.e., organic) BrC increased from 41% at 330 nm to 59 % at 550 nm while during the photochemistry-dominated summer period, the water-insoluble BrC fraction decreased from 73% at 400 nm to 41% at 530 nm, possibly due to photobleaching in the presence of OH. The BB-related BrC aerosol was also characterized by higher aromaticity and increased molecular weights of organic components as evidenced by mass absorption efficiency (MAE) ratios (MAE<sub>250</sub>/MAE<sub>365</sub>). Overall, this study established that BrC is a significant component of light-absorbing aerosol in the eastern IGP and that BrC optical properties may vary significantly in this region depending on the relative dominance of aerosol emissions and atmospheric processes.</p>


2014 ◽  
Vol 14 (20) ◽  
pp. 10989-11010 ◽  
Author(s):  
X. Wang ◽  
C. L. Heald ◽  
D. A. Ridley ◽  
J. P. Schwarz ◽  
J. R. Spackman ◽  
...  

Abstract. Atmospheric black carbon (BC) is a leading climate warming agent, yet uncertainties on the global direct radiative forcing (DRF) remain large. Here we expand a global model simulation (GEOS-Chem) of BC to include the absorption enhancement associated with BC coating and separately treat both the aging and physical properties of fossil-fuel and biomass-burning BC. In addition we develop a global simulation of brown carbon (BrC) from both secondary (aromatic) and primary (biomass burning and biofuel) sources. The global mean lifetime of BC in this simulation (4.4 days) is substantially lower compared to the AeroCom I model means (7.3 days), and as a result, this model captures both the mass concentrations measured in near-source airborne field campaigns (ARCTAS, EUCAARI) and surface sites within 30%, and in remote regions (HIPPO) within a factor of 2. We show that the new BC optical properties together with the inclusion of BrC reduces the model bias in absorption aerosol optical depth (AAOD) at multiple wavelengths by more than 50% at AERONET sites worldwide. However our improved model still underestimates AAOD by a factor of 1.4 to 2.8 regionally, with the largest underestimates in regions influenced by fire. Using the RRTMG model integrated with GEOS-Chem we estimate that the all-sky top-of-atmosphere DRF of BC is +0.13 Wm−2 (0.08 Wm−2 from anthropogenic sources and 0.05 Wm−2 from biomass burning). If we scale our model to match AERONET AAOD observations we estimate the DRF of BC is +0.21 Wm−2, with an additional +0.11 Wm−2 of warming from BrC. Uncertainties in size, optical properties, observations, and emissions suggest an overall uncertainty in BC DRF of −80%/+140%. Our estimates are at the lower end of the 0.2–1.0 Wm−2 range from previous studies, and substantially less than the +0.6 Wm−2 DRF estimated in the IPCC 5th Assessment Report. We suggest that the DRF of BC has previously been overestimated due to the overestimation of the BC lifetime (including the effect on the vertical profile) and the incorrect attribution of BrC absorption to BC.


2018 ◽  
Vol 18 (1) ◽  
pp. 405-425 ◽  
Author(s):  
Huizheng Che ◽  
Bing Qi ◽  
Hujia Zhao ◽  
Xiangao Xia ◽  
Thomas F. Eck ◽  
...  

Abstract. Aerosol pollution in eastern China is an unfortunate consequence of the region's rapid economic and industrial growth. Here, sun photometer measurements from seven sites in the Yangtze River Delta (YRD) from 2011 to 2015 were used to characterize the climatology of aerosol microphysical and optical properties, calculate direct aerosol radiative forcing (DARF) and classify the aerosols based on size and absorption. Bimodal size distributions were found throughout the year, but larger volumes and effective radii of fine-mode particles occurred in June and September due to hygroscopic growth and/or cloud processing. Increases in the fine-mode particles in June and September caused AOD440 nm > 1.00 at most sites, and annual mean AOD440 nm values of 0.71–0.76 were found at the urban sites and 0.68 at the rural site. Unlike northern China, the AOD440 nm was lower in July and August (∼ 0.40–0.60) than in January and February (0.71–0.89) due to particle dispersion associated with subtropical anticyclones in summer. Low volumes and large bandwidths of both fine-mode and coarse-mode aerosol size distributions occurred in July and August because of biomass burning. Single-scattering albedos at 440 nm (SSA440 nm) from 0.91 to 0.94 indicated particles with relatively strong to moderate absorption. Strongly absorbing particles from biomass burning with a significant SSA wavelength dependence were found in July and August at most sites, while coarse particles in March to May were mineral dust. Absorbing aerosols were distributed more or less homogeneously throughout the region with absorption aerosol optical depths at 440 nm ∼ 0.04–0.06, but inter-site differences in the absorption Angström exponent indicate a degree of spatial heterogeneity in particle composition. The annual mean DARF was −93 ± 44 to −79 ± 39 W m−2 at the Earth's surface and ∼ −40 W m−2 at the top of the atmosphere (for the solar zenith angle range of 50 to 80∘) under cloud-free conditions. The fine mode composed a major contribution of the absorbing particles in the classification scheme based on SSA, fine-mode fraction and extinction Angström exponent. This study contributes to our understanding of aerosols and regional climate/air quality, and the results will be useful for validating satellite retrievals and for improving climate models and remote sensing algorithms.


Atmosphere ◽  
2021 ◽  
Vol 12 (2) ◽  
pp. 276
Author(s):  
Ye Tao ◽  
Ning Sun ◽  
Xudong Li ◽  
Zhuzi Zhao ◽  
Shuaishuai Ma ◽  
...  

The chemical and optical properties and sources of atmospheric PM2.5 humic-like substances (HULIS) were investigated from October to December 2016 in both industrial and suburban areas in Changzhou, China, during polluted and fair days. The average PM2.5 concentration in the industrial region was 113.06 (±64.3) μg m−3, higher than 85.27 (±41.56) μg m−3 at the suburban site. The frequency of polluted days was significantly higher in the industrial region. In contrast, the chemical compositions of PM2.5 at the two sampling sites exhibited no statistically significant differences. Rapidly increased secondary inorganic ions (SNA = NH4+ + SO42− + NO3−) concentrations suggested secondary formation played an important role in haze formation. The daily mean concentration of humic-like substance (HULIS) was 1.8–1.9 times that of HULIS-C (the carbon content of HULIS). Our results showed that HULIS accounted for a considerable fraction of PM2.5 (industrial region: 6.3% vs. suburban region: 9.4%). There were no large differences in the mass ratios of HULIS-C/WSOC at the two sites (46% in the industrial region and 52% in the suburban region). On average, suburban HULIS-C constituted 35.1% of organic carbon (OC), higher than that (21.1%) in the industrial region. Based on different MAE (mass absorption efficiency) values under different pollution levels, we can infer that the optical properties of HULIS varied with PM levels. Moreover, our results showed no distinct difference in E2/E3 (the ratio of light absorbance at 250 nm to that at 365 nm) and AAE300–400 (Absorption Angstrom Exponent at 300–400 nm) for HULIS and WSOC. the MAE365 (MAE at 365 nm) value of HULIS-C was different under three PM2.5 levels (low: PM2.5 < 75 μg m−3, moderate: PM2.5 = 75–150 μg m−3, high: PM2.5 > 150 μg m−3), with the highest MAE365 value on polluted days in the industrial region. Strong correlations between HULIS-C and SNA revealed that HULIS might be contributed from secondary formation at both sites. In addition, good correlations between HULIS-C with K+ in the industrial region implied the importance of biomass burning to PM2.5-bound HULIS. Three common sources of HULIS-C (i.e., vehicle emissions, biomass burning, and secondary aerosols) were identified by positive matrix factorization (PMF) for both sites, but the contributions were different, with the largest contribution from biomass burning in the industrial region and secondary sources in the suburban region, respectively. The findings presented here are important in understanding PM2.5 HULIS chemistry and are valuable for future air pollution control measures.


2021 ◽  
Vol 11 (4) ◽  
pp. 1434
Author(s):  
Chang Hoon Jung ◽  
Sang Hee Han ◽  
Ji Yi Lee ◽  
Yong Pyo Kim

In this study, the source-based optical properties of polydisperse carbonaceous aerosols were determined from PM2.5 concentrations measured at a Global Atmospheric Watch station in South Korea. The extinction and absorption coefficients of carbonaceous aerosols were calculated using the Mie theory and assuming a lognormal size distribution. Based on the mass concentration from the EPA’s Positive Matrix Factorization (PMF) receptor model, which considers five source identification and apportionment factors (biogenic source, local biomass burning, secondary organic aerosol, transported biomass burning, and mixed sources), the source-based size-resolved mass extinction and absorption efficiencies were estimated for each source using a multilinear regression model. The results show that the source-based optical properties depend on the aerosol size and physicochemical characteristics of the chemical compounds. The long-range transport of biomass burning (LBB) aerosol, which has a mass concentration of 20%, holds a 12.1–23.1% total extinction efficiency—depending on the size and refractive index—in the range of 0.1–0.5 μm in geometric mean diameter and humic-like substances (HULIS) imaginary refractive index of 0.006–0.3. Biogenic sources of aerosols with small diameters have higher mass absorption efficiencies (MAE) than other sources, depending on the size and refractive index.


2014 ◽  
Vol 14 (11) ◽  
pp. 17527-17583 ◽  
Author(s):  
X. Wang ◽  
C. L. Heald ◽  
D. A. Ridley ◽  
J. P. Schwarz ◽  
J. R. Spackman ◽  
...  

Abstract. Atmospheric black carbon (BC) is a leading climate warming agent, yet uncertainties on the global direct radiative forcing (DRF) remain large. Here we expand a global model simulation (GEOS-Chem) of BC to include the absorption enhancement associated with BC coating and separately treat both the aging and physical properties of fossil fuel and biomass burning BC. In addition we develop a global simulation of Brown Carbon (BrC) from both secondary (aromatic) and primary (biomass burning and biofuel) sources. The global mean lifetime of BC in this simulation (4.4 days) is substantially lower compared to the AeroCom I model means (7.3 days), and as a result, this model captures both the mass concentrations measured in near-source airborne field campaigns (ARCTAS, EUCAARI) and surface sites within 30%, and in remote regions (HIPPO) within a factor of two. We show that the new BC optical properties together with the inclusion of BrC reduces the model bias in Absorption Aerosol Optical Depth (AAOD) at multiple wavelengths by more than 50% at AERONET sites worldwide. However our improved model still underestimates AAOD by a factor of 1.4 to 2.8 regionally, with largest underestimates in regions influenced by fire. Using the RRTMG model integrated with GEOS-Chem we estimate that the all-sky top-of-atmosphere DRF of BC is +0.13 W m−2 (0.08 W m−2 from anthropogenic sources and 0.05 W m−2 from biomass burning). If we scale our model to match AERONET AAOD observations we estimate the DRF of BC is +0.21 W m−2, with an additional +0.11 W m−2 of warming from BrC. Uncertainties in size, optical properties, observations, and emissions suggest an overall uncertainty in BC DRF of −80% / +140%. Our estimates are at the lower end of the 0.2–1.0 W m−2 range from previous studies, and substantially less than the +0.6 W m−2 DRF estimated in the IPCC 5th Assessment Report. We suggest that the DRF of BC has previously been overestimated due to the overestimation of the BC lifetime and the incorrect attribution of BrC absorption to BC.


2019 ◽  
Author(s):  
Yicheng Shen ◽  
Aki Virkkula ◽  
Aijun Ding ◽  
Krista Luoma ◽  
Helmi Keskinen ◽  
...  

Abstract. The concentration of cloud condensation nuclei (CCN) is an essential parameter affecting aerosol-cloud interactions within warm clouds. Long-term CCN number concentration (NCCN) data are scarce, there are a lot more data on aerosol optical properties (AOPs). It is therefore valuable to derive parameterizations for estimating NCCN from AOP measurements. Such parameterizatios have been made earlier, in the present work a new one is presented. The relationships between AOPs, NCCN and particle number size distributions were investigated based on in-situ measurement data from six stations in very different environments around the world. The parameterization derived here depends on the scattering Ångström exponent (SAE), backscatter fraction (BSF) and total scattering coefficient (σsp) of PM10 particles. The analysis showed that the dependence of NCCN on supersaturation SS% is logarithmic: NCCN ≈ ((287 ± 45)SAE10ln(SS%/(0.093 ± 0.006))(BSF − BSFmin) + (5.2 ± 3.3))σsp. At the lowest supersaturations of each site (SS% ≈ 0.1) the average bias, defined as the ratio of the AOP-derived and measured NCCN varied from ~ 0.7 to ~ 1.5 at most sites except at a Himalayan site where bias was > 4. At SS% > 0.3 the average bias ranged from ~ 0.7 to ~ 1.3 at all sites. In other words, at SS% > 0.3 NCCN was estimated with an average uncertainty of approximately 30 % by using nephelometer data. The squared correlation coefficients between the AOP-derived and measured NCCN varied from ~ 0.5 to ~ 0.8. The coefficients of the parameterization derived for the different sites were linearly related to each other. To study the explanation of this, lognormal unimodal particle size distributions were generated and NCCN and AOPs were calculated. The simulation yielded similar relationships between the coefficients as in the field data. It also showed that the relationships of the coefficients are affected by the geometric mean diameter and width of the size distribution and the activation diameter.


2015 ◽  
Vol 15 (10) ◽  
pp. 5429-5442 ◽  
Author(s):  
E. Giannakaki ◽  
A. Pfüller ◽  
K. Korhonen ◽  
T. Mielonen ◽  
L. Laakso ◽  
...  

Abstract. Raman lidar data obtained over a 1 year period has been analysed in relation to aerosol layers in the free troposphere over the Highveld in South Africa. In total, 375 layers were observed above the boundary layer during the period 30 January 2010 to 31 January 2011. The seasonal behaviour of aerosol layer geometrical characteristics, as well as intensive and extensive optical properties were studied. The highest centre heights of free-tropospheric layers were observed during the South African spring (2520 ± 970 m a.g.l., also elsewhere). The geometrical layer depth was found to be maximum during spring, while it did not show any significant difference for the rest of the seasons. The variability of the analysed intensive and extensive optical properties was high during all seasons. Layers were observed at a mean centre height of 2100 ± 1000 m with an average lidar ratio of 67 ± 25 sr (mean value with 1 standard deviation) at 355 nm and a mean extinction-related Ångström exponent of 1.9 ± 0.8 between 355 and 532 nm during the period under study. Except for the intensive biomass burning period from August to October, the lidar ratios and Ångström exponents are within the range of previous observations for urban/industrial aerosols. During Southern Hemispheric spring, the biomass burning activity is clearly reflected in the optical properties of the observed free-tropospheric layers. Specifically, lidar ratios at 355 nm were 89 ± 21, 57 ± 20, 59 ± 22 and 65 ± 23 sr during spring (September–November), summer (December–February), autumn (March–May) and winter (June–August), respectively. The extinction-related Ångström exponents between 355 and 532 nm measured during spring, summer, autumn and winter were 1.8 ± 0.6, 2.4 ± 0.9, 1.8 ± 0.9 and 1.8 ± 0.6, respectively. The mean columnar aerosol optical depth (AOD) obtained from lidar measurements was found to be 0.46 ± 0.35 at 355 nm and 0.25 ± 0.2 at 532 nm. The contribution of free-tropospheric aerosols on the AOD had a wide range of values with a mean contribution of 46%.


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