scholarly journals Light absorption by organic carbon from wood combustion

2010 ◽  
Vol 10 (4) ◽  
pp. 1773-1787 ◽  
Author(s):  
Y. Chen ◽  
T. C. Bond
Keyword(s):  
Organic Carbon ◽  
Radiative Transfer ◽  
Absorption Spectra ◽  
Light Absorption ◽  
Radiative Forcing ◽  
Water Soluble ◽  
Clear Sky ◽  
Wood Temperature ◽  
Visible Wavelengths ◽  
Positive Direct

Abstract. Carbonaceous aerosols affect the radiative balance of the Earth by absorbing and scattering light. While black carbon (BC) is highly absorbing, some organic carbon (OC) also has significant absorption, especially at near-ultraviolet and blue wavelengths. To the extent that OC absorbs visible light, it may be a non-negligible contributor to positive direct aerosol radiative forcing. Quantification of that absorption is necessary so that radiative-transfer models can evaluate the net radiative effect of OC. In this work, we examine absorption by primary OC emitted from solid fuel pyrolysis. We provide absorption spectra of this material, which can be related to the imaginary refractive index. This material has polar character but is not fully water-soluble: more than 92% was extractable by methanol or acetone, compared with 73% for water and 52% for hexane. Water-soluble OC contributes to light absorption at both ultraviolet and visible wavelengths. However, a larger portion of the absorption comes from OC that is extractable only by methanol. Absorption spectra of water-soluble OC are similar to literature reports. We compare spectra for material generated with different wood type, wood size and pyrolysis temperature. Higher wood temperature is the main factor creating OC with higher absorption; changing wood temperature from a devolatilizing state of 210 °C to a near-flaming state of 360 °C causes about a factor of four increase in mass-normalized absorption at visible wavelengths. A clear-sky radiative transfer model suggests that, despite the absorption, both high-temperature and low-temperature OC result in negative top-of-atmosphere radiative forcing over a surface with an albedo of 0.19 and positive radiative forcing over bright surfaces. Unless absorption by real ambient aerosol is higher than that measured here, it probably affects global average clear-sky forcing very little, but could be important in energy balances over bright surfaces.

scholarly journals Light absorption by organic carbon from wood combustion

2009 ◽  
Vol 9 (5) ◽  
pp. 20471-20513 ◽  
Author(s):  
Y. Chen ◽  
T. C. Bond
Keyword(s):  
Organic Carbon ◽  
Light Absorption ◽  
Radiative Forcing ◽  
Water Soluble ◽  
Carbonaceous Aerosols ◽  
Radiative Balance ◽  
Near Ultraviolet ◽  
Water Soluble Organic Carbon ◽  
Soluble Organic Carbon ◽  
Visible Wavelengths

Abstract. Carbonaceous aerosols affect the radiative balance of the Earth by absorbing and scattering light. While BC is highly absorbing, some organic compounds also have significant absorption, which is greater at near-ultraviolet and blue wavelengths. To the extent that OC absorbs visible light, it may be a non-negligible contributor to direct aerosol radiative forcing. In this work, we examine absorption by primary OC emitted from solid fuel pyrolysis. We provide absorption spectra of this material, which can be related to the imaginary refractive index. This material has polar character but is not fully water-soluble: more than 92% was extractable by methanol or acetone, compared with 73% for water and 52% for hexane. Water-soluble organic carbon contributed to light absorption at both ultraviolet and visible wavelengths. However, a larger portion came from organic carbon that is extractable only by methanol. The spectra of water-soluble organic carbon are similar to others in the literature. We compared spectra for material generated with different wood type, wood size and pyrolysis temperature. Higher wood temperature is the main factor creating organic aerosol with higher absorption, causing about a factor of four increase in mass-normalized absorption at visible wavelengths. A simple model suggests that, despite the absorption, both high-temperature and low-temperature carbon have negative climate forcing over a surface with average albedo.

scholarly journals Sources and light absorption of water-soluble organic carbon aerosols in the outflow from northern China

2014 ◽  
Vol 14 (3) ◽  
pp. 1413-1422 ◽  
Author(s):  
E. N. Kirillova ◽  
A. Andersson ◽  
J. Han ◽  
M. Lee ◽  
Ö. Gustafsson
Keyword(s):  
Organic Carbon ◽  
Light Absorption ◽  
Radiative Forcing ◽  
Large Fraction ◽  
Northern China ◽  
Water Soluble ◽  
Cloud Formation ◽  
Carbonaceous Aerosols ◽  
Water Soluble Organic Carbon ◽  
Soluble Organic Carbon

Abstract. High loadings of anthropogenic carbonaceous aerosols in Chinese air influence the air quality for over one billion people and impact the regional climate. A large fraction (17–80%) of this aerosol carbon is water-soluble, promoting cloud formation and thus climate cooling. Recent findings, however, suggest that water-soluble carbonaceous aerosols also absorb sunlight, bringing additional direct and indirect climate warming effects, yet the extent and nature of light absorption by this water-soluble "brown carbon" and its relation to sources is poorly understood. Here, we combine source estimates constrained by dual carbon isotopes with light-absorption measurements of water-soluble organic carbon (WSOC) for a March 2011 campaign at the Korea Climate Observatory at Gosan (KCOG), a receptor station in SE Yellow Sea for the outflow from northern China. The mass absorption cross section at 365 nm (MAC365) of WSOC for air masses from N. China were in general higher (0.8–1.1 m2 g−1), than from other source regions (0.3–0.8 m2 g−1). However, this effect corresponds to only 2–10% of the radiative forcing caused by light absorption by elemental carbon. Radiocarbon constraints show that the WSOC in Chinese outflow had significantly higher fraction fossil sources (30–50%) compared to previous findings in S. Asia, N. America and Europe. Stable carbon (δ13C) measurements were consistent with aging during long-range air mass transport for this large fraction of carbonaceous aerosols.

scholarly journals TD-DFT Monitoring of the Absorption Spectra of Polycyclic Aromatic Hydrocarbons over the Basque Country, Spain

2021 ◽  
Vol 2 (4) ◽  
pp. 599-609
Author(s):  
Patricia González-Berdullas ◽  
Luís Pinto da Silva
Keyword(s):  
Polycyclic Aromatic Hydrocarbons ◽  
Absorption Spectra ◽  
Aromatic Hydrocarbons ◽  
Light Absorption ◽  
Radiative Forcing ◽  
Basque Country ◽  
Absorption Properties ◽  
Td Dft ◽  
Polycyclic Aromatic ◽  
Visible Wavelengths

Brown carbon is a type of carbonaceous aerosol with strong light absorption in the ultraviolet and visible wavelengths that leads to radiative forcing. However, it is difficult to correlate the chemical composition of brown carbon with its atmospheric light absorption properties, which translates into significant uncertainty. Thus, a time-dependent density functional theory (TD-DFT) approach was used to model the real-world absorption properties of 14 polycyclic aromatic hydrocarbons (PAHs) over three regions of the Basque Country (Spain): Bilbao, Urretxu, and Azpeitia. The data were corrected for atmospheric concentration. The results show that the absorption spectra over each region are qualitatively identical, with the absorption intensities being significantly higher over Bilbao than over Azpeitia and Urretxu. Furthermore, it was found that the light absorption by PAHs should be more relevant for radiative forcing when it occurs at UVA and (sub)visible wavelengths. Finally, among the 14 studied PAHs, benzo[b]fluoranthene, pyrene, fluoranthene, benzo[a]pyrene, and benzo[k]fluoranthene and benzoperylene were identified as the molecules with larger contributions to radiative forcing.

Spatial and temporal heterogeneity in aerosol radiative effects over ecological area in south China: Composition and transmission implications

2020 ◽  
Author(s):  
Ma Yining ◽  
Xin Jinyuan
Keyword(s):  
Organic Carbon ◽  
Radiative Forcing ◽  
Dry Season ◽  
Water Soluble ◽  
Chemical Components ◽  
Radiative Effects ◽  
Wet Season ◽  
Cooling Effects ◽  
Ecological Region ◽  
Aerosol Radiative

<p><strong>Abstract:</strong> Ecological region in southern China has been perennially affected by monsoon climate and anthropogenic emissions, resulting in complex aerosol components and frequent long-range transport. In this study, a Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model is applied to estimate aerosol radiative forcing (ARF) and multiple aerosol observation datasets is used to estimate the aerosol chemical components and optical properties. The aerosol loading and the radiative effects in the ecological region exhibited strong seasonal changes. The average major components (NH<sub>4</sub><sup>+</sup>, NO<sub>3</sub><sup>−</sup>, SO<sub>4</sub><sup>2−</sup>) in Total water soluble ionic (TWSI) ,organic carbon (OC) concentration, the ratio of organic carbon to element carbon (OC/EC) and biogenic secondary organic aerosol (BSOA) tracers were 3.20±1.22 μg·m<sup>-3</sup>, 2.19±1.39 μg·m<sup>-3</sup>, 3.17 and 74.00±35.23 ng·m<sup>-3 </sup>in the dry season and 2.22±0.91 μg·m<sup>-3</sup>, 3.14±1.62 μg·m<sup>-3</sup>, 7.13 and 186.34±113.82 ng·m<sup>-3</sup> in the wet season, respectively. The average radiative forcing at the top of atmosphere (TOA) is -11.73±11.36 W/m<sup>2</sup> and -0.41±10.08 W/m<sup>2</sup> in dry and wet season. When the aerosol single scattering albedo (SSA) less than 0.9, the retrieve frequency in wet season reached account for 75%. The increase of OC and BSOA transformed by forests in the wet season weaken the cooling effects. However, the dry season is mainly composed of anthropogenic inorganic aerosols, which enhances the scattering effect. The aerosol observation baseline also verified the seasonal variation of ARF in the ecological region. Driven by multiple factors such as meteorological conditions, emission sources, and the mixed state of particulate matter, the transport patterns of air masses in ecological area exhibits completely opposite affects to ARF.</p>

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 Measurement Report: Optical properties and sources of water-soluble brown carbon in Tianjin, North China: insights from organic molecular compositions

2022 ◽  
Author(s):  
Junjun Deng ◽  
Hao Ma ◽  
Xinfeng Wang ◽  
Shujun Zhong ◽  
Zhimin Zhang ◽  
...  
Keyword(s):  
Optical Properties ◽  
Biomass Burning ◽  
Light Absorption ◽  
Radiative Forcing ◽  
North China ◽  
Water Soluble ◽  
Formation Mechanisms ◽  
Chemical Compositions ◽  
Brown Carbon ◽  
Near Ultraviolet

Abstract. Brown carbon (BrC) aerosols exert vital impacts on climate change and atmospheric photochemistry due to their light absorption in the wavelength range from near-ultraviolet (UV) to visible light. However, the optical properties and formation mechanisms of ambient BrC remain poorly understood, limiting the estimation of their radiative forcing. In the present study, fine aerosols (PM2.5) were collected during 2016–2017 on a day/night basis over urban Tianjin, a megacity in North China, to obtain seasonal and diurnal patterns of atmospheric water-soluble BrC. There were obvious seasonal but no evident diurnal variations in light absorption properties of BrC. In winter, BrC showed much stronger light absorbing ability since mass absorption efficiency at 365 nm (MAE365) (1.54 ± 0.33 m2 g−1), which was 1.8 times larger than that (0.84 ± 0.22 m2 g−1) in summer. Direct radiative effects by BrC absorption relative to black carbon in the UV range were 54.3 ± 16.9 % and 44.6 ± 13.9 %, respectively. In addition, five fluorescent components in BrC, including three humic-like fluorophores and two protein-like fluorophores were identified with excitation-emission matrix fluorescence spectrometry and parallel factor (PARAFAC) analysis. The lowly-oxygenated components contributed more to winter and nighttime samples, while more-oxygenated components increased in summer and daytime samples. The higher humification index (HIX) together with lower biological index (BIX) and fluorescence index (FI) suggest that the chemical compositions of BrC were associated with a high aromaticity degree in summer and daytime due to photobleaching. Fluorescent properties indicate that wintertime BrC were predominantly affected by primary emissions and fresh secondary organic aerosol (SOA), while summer ones were more influenced by aging processes. Results of source apportionments using organic molecular compositions of the same set of aerosols reveal that fossil fuel combustion and aging processes, primary bioaerosol emission, biomass burning, and biogenic and anthropogenic SOA formation were the main sources of BrC. Biomass burning contributed much larger to BrC in winter and at nighttime, while biogenic SOA contributed more in summer and at daytime. Especially, our study highlights that primary bioaerosol emission is an important source of BrC in urban Tianjin in summer.

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.

Optical and chemical properties of wintertime light-absorbing aerosols in the eastern Indo-Gangetic Plain, India

2020 ◽  
Author(s):  
Supriya Dey ◽  
Archita Rana ◽  
Prashant Rawat ◽  
Sayantan Sarkar
Keyword(s):  
Organic Carbon ◽  
Light Absorption ◽  
Mass Concentration ◽  
Chemical Properties ◽  
Water Soluble ◽  
Chemical Extraction ◽  
Aerosol Formation ◽  
Gangetic Plain ◽  
Indo Gangetic Plain ◽  
And Chemical Properties

<p>Light-absorbing carbonaceous aerosols such as black and brown carbon (BC and BrC) and humic-like substances (HULIS) have pronounced effects on the earth’s radiative balance and tropospheric photochemistry. In India, large heterogeneities exist for BC and organic carbon (OC) emission inventories, which necessitates regionally-representative ground-based measurements. Such measurements are spatially scattered for BC, rare for BrC and non-existent for HULIS. This severely limits a robust understanding of the optical and chemical properties of these aerosols, and consequently, their climate effects. To address this issue, the present study reports optical and chemical properties of wintertime (December 2018-February 2019) BC, BrC and HULIS at a rural receptor site in the highly polluted eastern Indo-Gangetic Plain (IGP), India. A 7 wavelength aethalometer was deployed to measure time-resolved BC mass concentration, and absorption coefficients (b<sub>abs</sub>) and Angstrom exponent (AE) of BrC. Separation of aqueous and organic BrC (BrC<sub>aq</sub> and BrC<sub>org</sub>) and HULIS fractions via a multi-step chemical extraction procedure followed by optical measurements (UV-Vis, fluorescence and FT-IR), and supplementary measurements of OC, water-soluble organic carbon (WSOC) and ionic species led to better insights into the potential chromophore composition and their relative importance in constraining aerosol optical properties.</p><p>The daily averaged BC mass concentration was 15.4±9.5 μg m<sup>-3</sup> during winter, where the biomass burning (BB) contribution was 25±5%. The diurnal profile of BC<sub>BB</sub> and BrC light absorption coefficient (b<sub>abs_BrC</sub>) showed a prominent morning peak (0700-0800 H) characterized by mixed fossil fuel and biofuel emission and a gradual increase towards night due to enhanced primary BB emission from cooking activities and lowering of the mixing depth. The regionally transported BB plume from northwestern IGP contributed substantial BC and BrC to this receptor location in the eastern end of the corridor, which was supported by concentration-weighted air mass trajectories (CWTs).</p><p>The BrC<sub>org</sub> light absorption at 365 nm (b<sub>abs_BrC_org</sub>) was almost 2 times compared to that of BrC<sub>aq</sub> (b<sub>abs_BrC_aq</sub>) (36±7.1 vs 18.3±4.3 Mm<sup>-1</sup>), which suggested a dominance of non-polar polyconjugated BrC chromophores. This was also supported by the increasing trend of water-insoluble BrC from 49±10% at 365 nm to 64±21% at 550 nm, with averaged contributions of 49±8% at 300-400 nm and 67±9% at 400-550 nm, respectively. A strong correlation between WSOC and NO<sub>3</sub><sup>- </sup>(r=0.78, p<0.01) and WSOC and NH<sub>4</sub><sup>+</sup> (r=0.63, p<0.01) indicated the possibility of nighttime secondary organic aerosol formation. A prominent fluorescence peak at ~409 nm for BrC<sub>aq </sub>confirmed the presence of HULIS, and b<sub>abs_BrC_aq</sub> was dominated by the low-polarity HULIS-n fraction. AE of individual HULIS fractions increased by 7-36% towards the more polar HULIS-a and highly-polar water-soluble organic matter (HPWSOM) compared to the less polar HULIS-n for the 300-700 nm range. Distinct FTIR peaks at 3400 cm<sup>-1</sup>, 1710 cm<sup>-1</sup> and 1643 cm<sup>-1</sup> suggested abundance of C-H, C=O and C=C functional groups, respectively, in the BrC chromophores. Overall, it appeared that the regionally transported BB plume significantly enriches BrC and HULIS in the eastern part of the IGP corridor.   </p>

Sign in / Sign up

Export Citation Format

Share Document