scholarly journals The influence of photochemical aging on light absorption of atmospheric black carbon and aerosol single-scattering albedo

2018 ◽  
Vol 18 (23) ◽  
pp. 16829-16844 ◽  
Author(s):  
Xuezhe Xu ◽  
Weixiong Zhao ◽  
Xiaodong Qian ◽  
Shuo Wang ◽  
Bo Fang ◽  
...  
Keyword(s):  
Black Carbon ◽  
Light Absorption ◽  
Radiative Forcing ◽  
Climate Models ◽  
Complex Refractive Index ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Rural Site ◽  
Diurnal Variability ◽  
Photochemical Aging

Abstract. Coating enhancement of black carbon (BC) light absorption (Eabs) is a large uncertainty in modelling direct radiative forcing (DRF) by BC. Reported Eabs values after atmospheric aging vary widely and the mechanisms responsible for enhancing BC absorption remain elusive. Here, we report on the direct field measurement of size-resolved mixing state, Eabs, and aerosol single-scattering albedo (SSA) at λ = 532 nm at a rural site in east China from June to July 2016. Strong diurnal variability of Eabs, SSA, and Ox (Ox = NO2 + O3, a proxy for atmospheric photochemical aging) was observed. A method that combined Eabs and SSA was developed to retrieve the fraction contribution of BC absorption (fBC), lensing-driven enhancement (fLens), as well as the fractional contribution of coating absorption (fraction absorption contribution (fShell), the coated shell diameter (DShell) and the imaginary part of the complex refractive index (CRI) of the shell (kShell)). Parameterization of Eabs and SSA captures much of the influence of BC coating and the particle absorption. In our measurements at this site, the results showed that the absorption amplification depended on the coating thickness and the absorption of coating materials, and photochemistry plays a role in modifying the absorption of BC-containing particles. The lensing-driven enhancement was reduced by light absorption of the shell. One implication of these findings is that the contribution of light-absorbing organic compounds (brown carbon, BrC) at a longer aging time should be included in climate models.

scholarly journals Influence of photochemical aging on light absorption of atmospheric black carbon and aerosol single scattering albedo

2018 ◽  
Author(s):  
Xuezhe Xu ◽  
Weixiong Zhao ◽  
Xiaodong Qian ◽  
Shuo Wang ◽  
Bo Fang ◽  
...  
Keyword(s):  
Growth Rate ◽  
Black Carbon ◽  
Light Absorption ◽  
Radiative Forcing ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Rural Site ◽  
Absorption Enhancement ◽  
Diurnal Variability ◽  
Photochemical Aging

Abstract. Coating enhancement of black carbon (BC) light absorption (Eabs) is a large uncertainty in modelling direct radiative forcing (DRF) by BC. Reported Eabs values after atmospheric aging vary widely and the mechanisms responsible for enhancing BC absorption remain elusive. Here, we report on the direct field measurement of size-resolved mixing state, Eabs and aerosol single scattering albedo (SSA) at λ = 532 nm at a rural site in East China from June to July 2016. Strong diurnal variability of Eabs, SSA, and Ox (Ox = NO2 + O3, a proxy for atmospheric photochemical aging) was observed. A three-stage absorption enhancement process for collapsed semispherical to fully compact spherical morphology BC with photochemical aging was suggested. For Ox below 35 ppbv, Eabs increased slowly with Ox mixing ratio and ranged from 2.0 to 2.2 (with a growth rate of ~ 0.03 ppbv−1). Eabs was stable (Eabs = 2.26 ± 0.06) between 35 to 50 ppbv Ox. Thirdly, for Ox levels above 50 ppbv, Eabs grew rapidly from 2.3 to 2.8 (at a growth rate of ~ 0.18 ppbv−1). A method that combined Eabs and SSA was developed to retrieve the fraction contribution of BC absorption (fBC), lensing driven enhancement (fLens), as well as the fractional contribution of coating absorption (fraction absorption contribution (fShell), the coated shell diameter (DShell) and the imaginary part of the complex refractive index (CRI) of the shell (kShell)). Parameterization of Eabs and SSA captures much of the influence of BC coating and the particle absorption, and provides a plausible new method to better constrain the contribution of BC to the DRF. In our measurements at this site, the absorption amplification depended mainly on the coating thickness and the absorption of coating materials. The lensing driven enhancement was reduced by light absorption of the shell. Our observations highlight the crucial role of photochemical processes in modifying the absorption of BC-containing particles. One implication of these findings is that the contribution of light-absorbing organic compounds (Brown carbon, BrC) at longer aging time should be included in climate models.

scholarly journals Vertical profiles of light absorption and scattering associated with black-carbon particle fractions in the springtime Arctic above 79° N

2019 ◽  
Author(s):  
W. Richard Leaitch ◽  
John K. Kodros ◽  
Megan D. Willis ◽  
Sarah Hanna ◽  
Hannes Schulz ◽  
...  
Keyword(s):  
Optical Properties ◽  
Absorption Coefficient ◽  
Black Carbon ◽  
Light Absorption ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
The Arctic ◽  
Vertical Profiles ◽  
Near Surface ◽  
Arctic Atmosphere

Abstract. Despite the potential importance of black carbon (BC) to radiative forcing of the Arctic atmosphere, vertically-resolved measurements of the particle light scattering coefficient (Bsp) and light absorption coefficient (Bap) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80oN. Here, relationships among vertically-distributed aerosol optical properties Bap, Bsp, and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9oN and 83.4oN from near the surface to 500 hPa. Airborne data collected during April, 2015, are combined with ground-based observations from the observatory at Alert, Nunavut and simulations from the GEOS-Chem-TOMAS model (Kodros et al., 2018) to increase our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for Bsp less than 15 Mm-1, which represent 98% of the observed Bsp, because the single scattering albedo (SSA) has a tendency to be lower at lower Bsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m2 g-1, the average BC mass absorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two averaged modelled MAC values (9.5 m2 g-1 and 7.0 m2 g-1) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC and possible differences in BC microphysics and morphologies between the observations and model. We present Bap and SSA based on the assumption that Bap is overestimated in the observations in addition to the assumption that the higher MAC is explained. Median values of the measured Bap, rBC and organic component of particles all increase by a factor of 1.8±0.1 going from near-surface to 750 hPa, and values higher than the surface persist to 600 hPa. Modelled BC, organics, and Bap agree with the near-surface measurements, but do not reproduce the higher values observed between 900 hPa and 600 hPa. The differences between modelled and observed optical properties follow the same trend as the differences between the modelled and observed concentrations of the carbonaceous components (black and organic). Some discrepancies in the model may be due to the use of a relatively low imaginary refractive index of BC as well as by the ejection of biomass burning particles only into the boundary layer at sources. For the assumption of the higher observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of Bsp <15 Mm-1. The large uncertainties in measuring optical properties and BC as well as the large differences between measured and modelled values, here and in the literature, argue for improved measurements of BC and light absorption by BC as well as more vertical profiles of aerosol chemistry, microphysics, and other optical properties in the Arctic.

scholarly journals Characterisation of episodic aerosol types over the Australian continent

2009 ◽  
Vol 9 (6) ◽  
pp. 1943-1956 ◽  
Author(s):  
Y. Qin ◽  
R. M. Mitchell
Keyword(s):  
Cluster Analysis ◽  
Optical Properties ◽  
Radiative Forcing ◽  
Climate Models ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Back Trajectory ◽  
Enhanced Absorption ◽  
Australian Continent ◽  
Aerosol Types

Abstract. Classification of Australian continental aerosol types resulting from episodes of enhanced source activity, such as smoke plumes and dust outbreaks, is carried out via cluster analysis of optical properties obtained from inversion of sky radiance distributions at Australian aerosol ground stations using data obtained over the last decade. The cluster analysis distinguishes four significant classes, which are identified on the basis of their optical properties and provenance as determined by satellite imagery and back-trajectory analysis. The four classes are identified respectively as aged smoke, fresh smoke, coarse dust and a super-absorptive aerosol. While the first three classes show similarities with comparable aerosol types identified elsewhere, the super-absorptive aerosol has no obvious foreign prototype. The class identified as coarse dust shows a prominent depression in single scattering albedo in the blue spectral region due to absorption by hematite, which is shown to be more abundant in central Australian dust relative to the "dust belt"of the Northern Hemisphere. The super-absorptive class is distinctive in view of its very low single scattering albedo (~0.7 at 500 nm) and variable enhanced absorption at 440 nm. The strong absorption by this aerosol requires a high black carbon content while the enhanced blue-band absorption may derive from organic compounds emitted during the burning of specific vegetation types. This aerosol exerts a positive radiative forcing at the top of atmosphere (TOA), with a large deposition of energy in the atmosphere per unit aerosol optical depth. This contrasts to the other three classes where the TOA forcing is negative. Optical properties of the four types will be used to improve the representation of Australian continental aerosol in climate models, and to enhance the accuracy of satellite-based aerosol retrievals over Australia.

scholarly journals Enhancement of snow albedo reduction and radiative forcing due to coated black carbon in snow

2021 ◽  
Vol 15 (5) ◽  
pp. 2255-2272
Author(s):  
Wei Pu ◽  
Tenglong Shi ◽  
Jiecan Cui ◽  
Yang Chen ◽  
Yue Zhou ◽  
...  
Keyword(s):  
Black Carbon ◽  
Light Absorption ◽  
Radiative Forcing ◽  
Climate Models ◽  
Northern China ◽  
Climate Impact ◽  
Arctic Sea Ice ◽  
The Arctic ◽  
Core Shell ◽  
Snow Albedo

Abstract. When black carbon (BC) is mixed internally with other atmospheric particles, the BC light absorption effect is enhanced. This study explicitly resolved the optical properties of coated BC in snow based on the core / shell Mie theory and the Snow, Ice, and Aerosol Radiative (SNICAR) model. Our results indicated that the BC coating effect enhances the reduction in snow albedo by a factor ranging from 1.1–1.8 for a nonabsorbing shell and 1.1–1.3 for an absorbing shell, depending on the BC concentration, snow grain radius, and core / shell ratio. We developed parameterizations of the BC coating effect for application to climate models, which provides a convenient way to accurately estimate the climate impact of BC in snow. Finally, based on a comprehensive set of in situ measurements across the Northern Hemisphere, we determined that the contribution of the BC coating effect to snow light absorption exceeds that of dust over northern China. Notably, high enhancements of snow albedo reduction due to the BC coating effect were found in the Arctic and Tibetan Plateau, suggesting a greater contribution of BC to the retreat of Arctic sea ice and Tibetan glaciers.

scholarly journals Vertical profiles of light absorption and scattering associated with black carbon particle fractions in the springtime Arctic above 79° N

2020 ◽  
Vol 20 (17) ◽  
pp. 10545-10563 ◽  
Author(s):  
W. Richard Leaitch ◽  
John K. Kodros ◽  
Megan D. Willis ◽  
Sarah Hanna ◽  
Hannes Schulz ◽  
...  
Keyword(s):  
Optical Properties ◽  
Absorption Coefficient ◽  
Black Carbon ◽  
Light Absorption ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
The Arctic ◽  
Vertical Profiles ◽  
Near Surface ◽  
Arctic Atmosphere

Abstract. Despite the potential importance of black carbon (BC) for radiative forcing of the Arctic atmosphere, vertically resolved measurements of the particle light scattering coefficient (σsp) and light absorption coefficient (σap) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80∘ N. Here, relationships among vertically distributed aerosol optical properties (σap, σsp and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9 and 83.4∘ N from near the surface to 500 hPa. Airborne data collected during April 2015 are combined with ground-based observations from the observatory at Alert, Nunavut and simulations from the Goddard Earth Observing System (GEOS) model, GEOS-Chem, coupled with the TwO-Moment Aerosol Sectional (TOMAS) model (collectively GEOS-Chem–TOMAS; Kodros et al., 2018) to further our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for σsp less than 15 Mm−1, which represent 98 % of the observed σsp, because the single scattering albedo (SSA) has a tendency to be lower at lower σsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m2 g−1, the average BC mass absorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two averaged modelled MAC values (13.6 and 9.1 m2 g−1) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC, the presence of small amounts of dust and/or possible differences in BC microphysics and morphologies between the observations and model. In comparing the observations and simulations, we present σap and SSA, as measured, and σap∕2 and the corresponding SSA to encompass the lower modelled MAC that is more consistent with accepted MAC values. Median values of the measured σap, rBC and the organic component of particles all increase by a factor of 1.8±0.1, going from near-surface to 750 hPa, and values higher than the surface persist to 600 hPa. Modelled BC, organics and σap agree with the near-surface measurements but do not reproduce the higher values observed between 900 and 600 hPa. The differences between modelled and observed optical properties follow the same trend as the differences between the modelled and observed concentrations of the carbonaceous components (black and organic). Model-observation discrepancies may be mostly due to the modelled ejection of biomass burning particles only into the boundary layer at the sources. For the assumption of the observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of σsp<15 Mm−1. The large uncertainties in measuring optical properties and BC, and the large differences between measured and modelled values here and in the literature, argue for improved measurements of BC and light absorption by BC and more vertical profiles of aerosol chemistry, microphysics and other optical properties in the Arctic.

scholarly journals Enhancement of snow albedo reduction and radiative forcing due to coated black carbon in snow

2020 ◽  
Author(s):  
Wei Pu ◽  
Tenglong Shi ◽  
Jiecan Cui ◽  
Yang Chen ◽  
Yue Zhou ◽  
...  
Keyword(s):  
Black Carbon ◽  
Light Absorption ◽  
Radiative Forcing ◽  
Climate Models ◽  
Northern China ◽  
Climate Impact ◽  
Arctic Sea Ice ◽  
The Arctic ◽  
Core Shell ◽  
Snow Albedo

Abstract. When black carbon (BC) is internally mixed with other atmospheric particles, BC light absorption is effectively enhanced. This study is the first to explicitly resolve the optical properties of coated BC in snow, based on core/shell Mie theory and a snow, ice, and aerosol radiative model (SNICAR). Our results indicate that a "BC coating effect" enhances the reduction of snow albedo by a factor of 1.1–1.8 for a non-absorbing shell and 1.1–1.3 for an absorbing shell, depending on BC concentration, snow grain radius, and core/shell ratio. We develop parameterizations of the BC coating effect for application to climate models, which provides a convenient way to accurately estimate the climate impact of BC in snow. Finally, based on a comprehensive set of in situ measurements across the Northern Hemisphere, we find that the contribution of the BC coating effect to snow light absorption has exceeded that of dust over northern China. Notably, the high enhancements of snow albedo reductions by BC coating effect were found in the Arctic and Tibetan Plateau, suggesting a greater contribution of BC to the retreat of Arctic sea ice and Tibetan glaciers.

scholarly journals Characterisation of episodic aerosol types over the Australian continent

2008 ◽  
Vol 8 (6) ◽  
pp. 18803-18842 ◽  
Author(s):  
Y. Qin ◽  
R. M. Mitchell
Keyword(s):  
Cluster Analysis ◽  
Optical Properties ◽  
Radiative Forcing ◽  
Climate Models ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Back Trajectory ◽  
Enhanced Absorption ◽  
Australian Continent ◽  
Aerosol Types

Abstract. Classification of Australian continental aerosol types resulting from episodes of enhanced source activity, such as smoke plumes and dust outbreaks, is carried out via cluster analysis of microphysical properties obtained from inversion of sky radiance distributions at Australian aerosol ground stations using data obtained over the last decade. The cluster analysis distinguishes four significant classes, which are identified on the basis of their optical properties and provenance as determined by satellite imagery and back-trajectory analysis. The four classes are identified respectively as aged smoke, fresh smoke, coarse dust and a super-absorptive aerosol. While the first three classes show similarities with comparable aerosol types identified elsewhere, the super-absorptive aerosol has no obvious foreign prototype. The class identified as coarse dust shows a prominent depression in single scattering albedo in the blue spectral region due to absorption by hematite, which is shown to be more abundant in central Australian dust relative to the "dust belt" of the Northern Hemisphere. The super-absorptive class is distinctive in view of its very low single scattering albedo (~0.7 at 500 nm) and variable enhanced absorption at 440 nm. The strong absorption by this aerosol requires a high black carbon content while the enhanced blue-band absorption may derive from organic compounds emitted during the burning of specific vegetation types. This aerosol exerts a positive radiative forcing at the top of atmosphere (TOA), with a large deposition of energy in the atmosphere per unit aerosol optical depth. This contrasts to the other three classes where the TOA forcing is negative. Optical properties of the four types will be used to improve the representation of Australian continental aerosol in climate models, and to enhance the accuracy of satellite-based aerosol retrievals over Australia.

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