scholarly journals Size-resolved measurements of brown carbon and estimates of their contribution to ambient fine particle light absorption based on water and methanol extracts

2013 ◽  
Vol 13 (7) ◽  
pp. 18233-18276 ◽  
Author(s):  
J. Liu ◽  
M. Bergin ◽  
H. Guo ◽  
L. King ◽  
N. Kotra ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Light Absorption ◽  
Fine Particle ◽  
Elemental Carbon ◽  
Fine Particles ◽  
Water Soluble ◽  
Rural Site ◽  
Brown Carbon ◽  
Methanol Extracts ◽  
Carbon Absorption

Abstract. Light absorbing organic carbon, often termed brown carbon, has the potential to significantly contribute to the visible light absorption budget, particularly at shorter wavelengths. Currently, the relative contributions of particulate brown carbon to light absorption, as well as the sources of brown carbon are poorly understood. With this in mind field measurements were made at both urban (Atlanta), and rural (Yorkville) sites in Georgia. Measurements in Atlanta were made at both a central site and a road side site adjacent to a main highway near the city center. Fine particle brown carbon optical absorption is estimated based on Mie calculations using direct size resolved measurements of chromophores in filter extracts. Size-resolved atmospheric aerosol samples were collected using a cascade impactor and analyzed for water-soluble organic carbon (WSOC), organic and elemental carbon (OC and EC), and solution light absorption spectra of water and methanol extracts. Methanol extracts were more light-absorbing than water extracts for all size ranges and wavelengths. Absorption refractive indices of the organic extracts were calculated from solution measurements for a range of wavelengths and used with Mie theory to predict the light absorption by fine particles comprised of these components, under the assumption that brown carbon and other aerosol components were externally mixed. For all three sites, chromophores were predominately in the accumulation mode with an aerodynamic mean diameter of 0.5 μm, an optically effective size range resulting in predicted particle light absorption being a factor of 2 higher than bulk solution absorption. Fine particle absorption was also measured with a Multi-Angle Absorption Photometer (MAAP) and seven-wavelength Aethalometer. Scattering-corrected aethalometer and MAAP absorption were in good agreement at 670 nm and Mie-estimated absorption based on size-resolved EC data were within 30% of these optical instruments. When applied to solution measurements, at all sites, Mie-predicted brown carbon absorption at 350 nm contributed a significant fraction (20 to 40%) relative to total light absorption, with highest contributions at the rural site where organic to elemental carbon ratios were highest. Brown carbon absorption, however, was highest by the roadside site due to vehicle emissions. The multi-wavelength aethalometer did not detect brown carbon, having an absorption Ångstrom exponent near one. Although the results are within the estimated Aethalometer uncertainties, the direct measurement of brown carbon in solution definitively shows that it is present and this Mie analysis suggests it is optically important in the near UV range in both a rural and urban environment during summer when biomass burning emissions are low.

scholarly journals Size-resolved measurements of brown carbon in water and methanol extracts and estimates of their contribution to ambient fine-particle light absorption

2013 ◽  
Vol 13 (24) ◽  
pp. 12389-12404 ◽  
Author(s):  
J. Liu ◽  
M. Bergin ◽  
H. Guo ◽  
L. King ◽  
N. Kotra ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Light Absorption ◽  
Fine Particle ◽  
Elemental Carbon ◽  
Rural Site ◽  
Urban Site ◽  
Brown Carbon ◽  
Methanol Extracts ◽  
Direct Measurements ◽  
Carbon Absorption

Abstract. Light absorbing organic carbon, often called brown carbon, has the potential to significantly contribute to the visible light-absorption budget, particularly at shorter wavelengths. Currently, the relative contributions of particulate brown carbon to light absorption, as well as the sources of brown carbon, are poorly understood. With this in mind size-resolved direct measurements of brown carbon were made at both urban (Atlanta), and rural (Yorkville) sites in Georgia. Measurements in Atlanta were made at both a representative urban site and a road-side site adjacent to a main highway. Fine particle absorption was measured with a multi-angle absorption photometer (MAAP) and seven-wavelength Aethalometer, and brown carbon absorption was estimated based on Mie calculations using direct size-resolved measurements of chromophores in solvents. Size-resolved samples were collected using a cascade impactor and analyzed for water-soluble organic carbon (WSOC), organic and elemental carbon (OC and EC), and solution light-absorption spectra of water and methanol extracts. Methanol extracts were more light-absorbing than water extracts for all size ranges and wavelengths. Absorption refractive indices of the organic extracts were calculated from solution measurements for a range of wavelengths and used with Mie theory to predict the light absorption by fine particles comprised of these components, under the assumption that brown carbon and other aerosol components were externally mixed. For all three sites, chromophores were predominately in the accumulation mode with an aerodynamic mean diameter of 0.5 μm, an optically effective size range resulting in predicted particle light absorption being a factor of 2 higher than bulk solution absorption. Mie-predicted brown carbon absorption at 350 nm contributed a significant fraction (20 to 40%) relative to total light absorption, with the highest contributions at the rural site where organic to elemental carbon ratios were highest. Brown carbon absorption, however, was highest by the roadside site due to vehicle emissions. The direct size-resolved measurement of brown carbon in solution definitively shows that it is present and optically important in the near-UV range in both a rural and urban environment during the summer when biomass burning emissions are low. These results allow estimates of brown carbon aerosol absorption from direct measurements of chromophores in aerosol extracts.

scholarly journals Optical properties of elemental carbon and water-soluble organic carbon in Beijing, China

2011 ◽  
Vol 11 (2) ◽  
pp. 6221-6258
Author(s):  
Y. Cheng ◽  
K.-B. He ◽  
M. Zheng ◽  
F.-K. Duan ◽  
Y.-L. Ma ◽  
...  
Keyword(s):  
Optical Properties ◽  
Organic Carbon ◽  
Biomass Burning ◽  
Light Absorption ◽  
Elemental Carbon ◽  
Water Soluble ◽  
Brown Carbon ◽  
Sulphate Concentration ◽  
Water Soluble Organic Carbon ◽  
Soluble Organic Carbon

Abstract. The mass absorption cross-section (MAC) of elemental carbon (EC) in Beijing was quantified using a thermal-optical carbon analyzer and the influences of mixing state and sources of carbonaceous aerosol were investigated. The MAC measured at 632 nm was 29.0 and 32.0 m2 g−1 during winter and summer respectively. MAC correlated well with the organic carbon (OC) to EC ratio (R2 = 0.91) which includes important information about the extent of secondary organic aerosol (SOA) production, indicating the enhancement of MAC by coating with SOA. The extrapolated MAC value was 10.5 m2 g−1 when the OC to EC ratio is zero, which was 5.6 m2 g−1 after correction by the enhancement factor (1.87) caused by the artifacts associated with the "filter-based" methods. The MAC also increased with sulphate (R2 = 0.84) when the sulphate concentration was below 10 μg m−3, whereas MAC and sulphate were only weekly related when the sulphate concentration was above 10 μg m−3, indicating the MAC of EC was also enhanced by coating with sulphate. Based on a converting approach that accounts for the discrepancy caused by measurements methods of both light absorption and EC concentration, previously published MAC values were converted to the "equivalent MAC", which is the estimated value if using the same measurement methods as used in this study. The "equivalent MAC" was found to be much lower in the regions heavily impacted by biomass burning (e.g., India), probably due to the influence of brown carbon. Optical properties of water-soluble organic carbon (WSOC) in Beijing were also presented. Light absorption by WSOC exhibited strong wavelength (λ) dependence such that absorption varied approximately as λ−7, which was characteristic of the brown carbon spectra. The mass absorption efficiency (σabs) of WSOC (measured at 365 nm) was 1.83 and 0.70 m2 g−1 during winter and summer respectively. The seasonal pattern of σabs was attributed to the difference in the precursors of SOA, because WSOC in Beijing has been demonstrated to be strongly linked to SOA. Moreover, the σabs of WSOC in Beijing was much higher than results from the southeastern United States which were obtained using the same method as used in this study, perhaps due to the influence of biomass burning.

Light absorption properties of elemental carbon (EC) and water-soluble brown carbon (WS–BrC) in the Kathmandu Valley, Nepal: A 5-year study

2020 ◽  
Vol 261 ◽  
pp. 114239 ◽  
Author(s):  
Pengfei Chen ◽  
Shichang Kang ◽  
Lekhendra Tripathee ◽  
Kirpa Ram ◽  
Maheswar Rupakheti ◽  
...  
Keyword(s):  
Light Absorption ◽  
Elemental Carbon ◽  
Water Soluble ◽  
Kathmandu Valley ◽  
Absorption Properties ◽  
Brown Carbon

scholarly journals Fossil and non-fossil sources of organic carbon (OC) and elemental carbon (EC) in Göteborg, Sweden

2009 ◽  
Vol 9 (5) ◽  
pp. 1521-1535 ◽  
Author(s):  
S. Szidat ◽  
M. Ruff ◽  
N. Perron ◽  
L. Wacker ◽  
H.-A. Synal ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Elemental Carbon ◽  
Latin Hypercube Sampling ◽  
Water Soluble ◽  
Total Carbon ◽  
Rural Site ◽  
Urban Site ◽  
Winter Period ◽  
Back Trajectories ◽  
Wood Burning

Abstract. Particulate matter was collected at an urban site in Göteborg (Sweden) in February/March 2005 and in June/July 2006. Additional samples were collected at a rural site for the winter period. Total carbon (TC) concentrations were 2.1–3.6 μg m−3, 1.8–1.9 μg m−3, and 2.2–3.0 μg m−3 for urban/winter, rural/winter, and urban/summer conditions, respectively. Elemental carbon (EC), organic carbon (OC), water-insoluble OC (WINSOC), and water-soluble OC (WSOC) were analyzed for 14C in order to distinguish fossil from non-fossil emissions. As wood burning is the single major source of non-fossil EC, its contribution can be quantified directly. For non-fossil OC, the wood-burning fraction was determined independently by levoglucosan and 14C analysis and combined using Latin-hypercube sampling (LHS). For the winter period, the relative contribution of EC from wood burning to the total EC was >3 times higher at the rural site compared to the urban site, whereas the absolute concentrations of EC from wood burning were elevated only moderately at the rural compared to the urban site. Thus, the urban site is substantially more influenced by fossil EC emissions. For summer, biogenic emissions dominated OC concentrations most likely due to secondary organic aerosol (SOA) formation. During both seasons, a more pronounced fossil signal was observed for Göteborg than has previously been reported for Zurich, Switzerland. Analysis of air mass origin using back trajectories suggests that the fossil impact was larger when local sources dominated, whereas long-range transport caused an enhanced non-fossil signal. In comparison to other European locations, concentrations of levoglucosan and other monosaccharide anhydrides were low for the urban and the rural site in the area of Göteborg during winter.

scholarly journals Mass absorption efficiency of elemental carbon and water-soluble organic carbon in Beijing, China

2011 ◽  
Vol 11 (22) ◽  
pp. 11497-11510 ◽  
Author(s):  
Y. Cheng ◽  
K.-B. He ◽  
M. Zheng ◽  
F.-K. Duan ◽  
Z.-Y. Du ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Biomass Burning ◽  
Light Absorption ◽  
Elemental Carbon ◽  
Organic Aerosol ◽  
Absorption Efficiency ◽  
Water Soluble ◽  
Water Soluble Organic Carbon ◽  
Soluble Organic Carbon ◽  
Mass Absorption Efficiency

Abstract. The mass absorption efficiency (MAE) of elemental carbon (EC) in Beijing was quantified using a thermal-optical carbon analyzer. The MAE measured at 632 nm was 8.45±1.71 and 9.41±1.92 m2 g−1 during winter and summer respectively. The daily variation of MAE was found to coincide with the abundance of organic carbon (OC), especially the OC to EC ratio, perhaps due to the enhancement by coating with organic aerosol (especially secondary organic aerosol, SOA) or the artifacts resulting from the redistribution of liquid-like organic particles during the filter-based absorption measurements. Using a converting approach that accounts for the discrepancy caused by measurements methods of both light absorption and EC concentration, previously published MAE values were converted to the equivalent-MAE, which is the estimated value if using the same measurement methods as used in this study. The equivalent-MAE was found to be much lower in the regions heavily impacted by biomass burning (e.g., below 2.7 m2 g−1 for two Indian cities). Results from source samples (including diesel exhaust samples and biomass smoke samples) also demonstrated that emissions from biomass burning would decrease the MAE of EC. Moreover, optical properties of water-soluble organic carbon (WSOC) in Beijing were presented. Light absorption by WSOC exhibited strong wavelength (λ) dependence such that absorption varied approximately as λ−7, which was characteristic of the brown carbon spectra. The MAE of WSOC (measured at 365 nm) was 1.79±0.24 and 0.71±0.20 m2 g−1 during winter and summer respectively. The large discrepancy between the MAE of WSOC during winter and summer was attributed to the difference in the precursors of SOA such that anthropogenic volatile organic compounds (AVOCs) should be more important as the precursors of SOA in winter. The MAE of WSOC in Beijing was much higher than results from the southeastern United States which were obtained using the same method as used in this study, perhaps due to the stronger emissions of biomass burning in China.

scholarly journals Fossil and non-fossil sources of organic carbon (OC) and elemental carbon (EC) in Göteborg, Sweden

2008 ◽  
Vol 8 (4) ◽  
pp. 16255-16289 ◽  
Author(s):  
S. Szidat ◽  
M. Ruff ◽  
L. Wacker ◽  
H.-A. Synal ◽  
M. Hallquist ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Elemental Carbon ◽  
Latin Hypercube Sampling ◽  
Water Soluble ◽  
Rural Site ◽  
Urban Site ◽  
Winter Period ◽  
Back Trajectories ◽  
Relative Contribution ◽  
Wood Burning

Abstract. Particulate matter was collected at an urban site in Göteborg (Sweden) in February/March 2005 and in June/July 2006. Additional samples were collected at a rural site for the winter period. Elemental carbon (EC), organic carbon (OC), water-insoluble OC (WINSOC), and water-soluble OC (WSOC) were analyzed for 14C in order to distinguish fossil from non-fossil emissions. As wood burning is the single major source of non-fossil EC, its contribution can be quantified directly. For non-fossil OC, the wood burning fraction was determined independently by levoglucosan and 14C analysis and combined using Latin-hypercube sampling (LHS). For the winter period, the relative contribution of EC from wood burning to the total EC was >3 times higher at the rural site compared to the urban site, whereas the absolute concentrations of EC from wood burning were comparable at both sites. Thus, the urban site is substantially more influenced by fossil EC emissions. For summer, biogenic emissions dominated OC concentrations most likely due to secondary organic aerosol (SOA) formation. During both seasons, a more pronounced fossil signal was observed for Göteborg than has previously been reported for Zurich, Switzerland. Analysis of air mass origin using back trajectories suggests that the fossil impact was larger when local sources dominated, whereas long-range transport caused an enhanced non-fossil signal. In comparison to other European locations, concentrations of levoglucosan and other monosaccharide anhydrides were low for the urban and the rural site in the area of Göteborg during winter. The comparison of summer and winter results provides insight into the annual cycle of anthropogenic vs. biogenic contributions to the atmospheric aerosol.

scholarly journals Optical properties and molecular compositions of water-soluble and water-insoluble brown carbon (BrC) aerosols in Northwest China

2019 ◽  
Author(s):  
Jianjun Li ◽  
Qi Zhang ◽  
Gehui Wang ◽  
Jin Li ◽  
Can Wu ◽  
...  
Keyword(s):  
Light Absorption ◽  
Winter Season ◽  
Northwest China ◽  
Water Soluble ◽  
Rural Site ◽  
Radiation Balance ◽  
Absorption Coefficients ◽  
Brown Carbon ◽  
Average Mass ◽  
Guanzhong Basin

Abstract. Brown carbon (BrC) contributes significantly to aerosol light absorption, thus can affect the earth's radiation balance and atmospheric photochemical processes. In this study, we examined the light absorption properties and molecular compositions of water-soluble (WS) and water-insoluble (WI) BrC in PM2.5 collected from a rural site in the Guanzhong Basin – a highly polluted region in Northwest China. Both WS-BrC and WI-BrC showed elevated light absorption coefficients (Abs) in winter (4–7 times of those in summer) mainly attributed to enhanced emissions from residential biomass burning (BB) for heating. While the average mass absorption coefficients at 365 nm (MAC365) of WS-BrC were similar between daytime and nighttime in summer (0.99 ± 0.17 and 1.01 ± 0.18 m2 g−1, respectively), the average MAC365 of WI-BrC was more than a factor of 2 higher during daytime (2.45 ± 1.14 m2 g−1) than at night (1.18 ± 0.36 m2 g−1). This difference was mainly attributed to enhanced photochemical formation of WI-BrC species, such as oxygenated polycyclic aromatic hydrocarbons (OPAHs). In contrast, the MACs of WS-BrC and WI-BrC were generally similar in winter and both showed little diel differences. The Abs of WS-BrC correlated strongly with relative humidity, sulfate, and NO2, suggesting that aqueous-phase reactions is an important pathway for secondary BrC formation during the winter season in Northwest China. Nitrophenols on average contributed 2.44 ± 1.78 % of the Abs of WS-BrC in winter, but only 0.12 ± 0.03 % in summer due to faster photodegradation reactions. WS-BrC and WI-BrC were estimated to account for 0.83 ± 0.23 % and 0.53 ± 0.33 %, respectively, of the total down-welling solar radiation in the UV range in summer, and 1.67 ± 0.72 % and 2.07 ± 1.24 %, respectively, in winter. The total absorption by BrC in the UV region was about 55–79 % relative to the elemental carbon (EC) absorption.

Seasonal light absorption properties of water-soluble brown carbon in atmospheric fine particles in Nanjing, China

2018 ◽  
Vol 187 ◽  
pp. 230-240 ◽  
Author(s):  
Yanfang Chen ◽  
Xinlei Ge ◽  
Hui Chen ◽  
Xinchun Xie ◽  
Yuntao Chen ◽  
...  
Keyword(s):  
Light Absorption ◽  
Fine Particles ◽  
Water Soluble ◽  
Absorption Properties ◽  
Brown Carbon

scholarly journals Contributions of biomass/biofuel burning to organic aerosols and particulate matter in Tanzania, East Africa, based on analyses of ionic species, organic and elemental carbon, levoglucosan and mannosan

2013 ◽  
Vol 13 (20) ◽  
pp. 10325-10338 ◽  
Author(s):  
S. L. Mkoma ◽  
K. Kawamura ◽  
P. Q. Fu
Keyword(s):  
Particulate Matter ◽  
Organic Carbon ◽  
East Africa ◽  
Biomass Burning ◽  
Elemental Carbon ◽  
Dry Season ◽  
Water Soluble ◽  
Total Carbon ◽  
Rural Site ◽  
Pm2.5 And Pm10

Abstract. Atmospheric aerosol samples of PM2.5 and PM10 were collected at a rural site in Tanzania, East Africa, in 2011 during wet and dry seasons and were analysed for carbonaceous components, levoglucosan, mannosan and water-soluble inorganic ions. The contributions of biomass/biofuel burning to the organic carbon (OC) and particulate matter (PM) mass were estimated to be 46–52% and 87–13%, respectively. The mean mass concentrations of PM2.5 and PM10 were 28 ± 6 μg m−3 and 47 ± 8 μg m−3 in wet season, and 39 ± 10 μg m−3 and 61 ± 19 μg m−3 in dry season, respectively. Total carbon (TC) accounted for 16–19% of the PM2.5 mass and 13–15% of the PM10 mass. On average, 86 to 89% of TC in PM2.5 and 87 to 90% of TC in PM10 was OC, of which 67–72% and 63% was found to be water-soluble organic carbon (WSOC) in PM2.5 and PM10, respectively. We found that concentrations of levoglucosan and mannosan (specific organic tracers of pyrolysis of cellulose) well correlated with non-sea-salt potassium (nss-K+) (r2 = 0.56–0.75), OC (r2 = 0.75–0.96) and WSOC (r2 = 0.52–0.78). The K+ / OC ratios varied from 0.06 to 0.36 in PM2.5 and from 0.03 to 0.36 in PM10 with slightly higher ratios in dry season. Mean percent ratios of levoglucosan and mannosan to OC were found to be 3–4% for PM2.5 and PM10 in both seasons. We found lower levoglucosan / K+ ratios and higher K+ / EC (elemental carbon) ratios in the biomass-burning aerosols from Tanzania than those reported from other regions. This feature is consistent with the high levels of potassium reported in the soils of Morogoro, Tanzania, suggesting an importance of direct emission of potassium by soil resuspension although K+ is present mostly in fine particles. It is also likely that biomass burning of vegetation of Tanzania emits high levels of potassium that may be enriched in plant tissues. The present study demonstrates that emissions from mixed biomass- and biofuel-burning activities largely influence the air quality in Tanzania.

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