scholarly journals Simplifying the calculation of light scattering properties for black carbon fractal aggregates

2014 ◽  
Vol 14 (15) ◽  
pp. 7825-7836 ◽  
Author(s):  
A. J. A. Smith ◽  
R. G. Grainger
Keyword(s):  
Light Scattering ◽  
Black Carbon ◽  
Cross Sections ◽  
Asymmetry Parameter ◽  
Size Distributions ◽  
Fractal Aggregates ◽  
Lognormal Distributions ◽  
Spherical Models ◽  
Computationally Expensive ◽  
Scattering Cross Sections

Abstract. Black carbon fractal aggregates have complicated shapes that make the calculation of their optical properties particularly computationally expensive. Here, a method is presented to estimate fractal aggregate light scattering properties by optimising simplified models to full light scattering calculations. It is found that there are no possible spherical models (at any size or refractive index) that well represent the light scattering in the visible or near-thermal infrared. As such, parameterisations of the light scattering as a function of the number of aggregate particles is presented as the most pragmatic choice for modelling distributions of black carbon when the large computational overheads of rigorous scattering calculations cannot be justified. This parameterisation can be analytically integrated to provide light scattering properties for lognormal distributions of black carbon fractal aggregates and return extinction cross sections with 0.1% accuracy for typical black carbon size distributions. Scattering cross sections and the asymmetry parameter can be obtained to within 3%.

scholarly journals Simplifying the calculation of light scattering properties for black carbon fractal aggregates

2014 ◽  
Vol 14 (3) ◽  
pp. 3537-3562 ◽  
Author(s):  
A. J. A. Smith ◽  
R. G. Grainger
Keyword(s):  
Light Scattering ◽  
Black Carbon ◽  
Cross Sections ◽  
Asymmetry Parameter ◽  
Size Distributions ◽  
Fractal Aggregates ◽  
Normal Distributions ◽  
Spherical Models ◽  
Log Normal ◽  
Scattering Cross Sections

Abstract. Black carbon fractal aggregates have complicated shapes that make the calculation of their optical properties particularly computationally expensive. Here, a method is presented to estimate fractal aggregate light scattering properties by optimising simplified models to full light scattering calculations. It is found that there are no possible spherical models (at any size or refractive index) that well represent the light scattering in the visible, or near-thermal infrared. As such, parameterisations of the light scattering as a function of the number of aggregate particles is presented as the most pragmatic choice for modelling distributions of black carbon when the large computational overheads of rigorous scattering calculations cannot be justified. This parameterisation can be analytically integrated to provide light scattering properties for log-normal distributions of black carbon fractal aggregates and return extinction cross-sections with 0.1% accuracy for typical black carbon size distributions. Scattering cross-sections and the asymmetry parameter can be obtained to within 3%.

scholarly journals Optical properties of coated black carbon aggregates: numerical simulations, radiative forcing estimates, and size-resolved parameterization scheme

2021 ◽  
Vol 21 (17) ◽  
pp. 12989-13010
Author(s):  
Baseerat Romshoo ◽  
Thomas Müller ◽  
Sascha Pfeifer ◽  
Jorge Saturno ◽  
Andreas Nowak ◽  
...  
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Cross Sections ◽  
Asymmetry Parameter ◽  
Radiative Forcing ◽  
Single Scattering ◽  
Parameterization Scheme ◽  
Fractal Aggregates ◽  
Mobility Diameter ◽  
The Cross

Abstract. The formation of black carbon fractal aggregates (BCFAs) from combustion and subsequent ageing involves several stages resulting in modifications of particle size, morphology, and composition over time. To understand and quantify how each of these modifications influences the BC radiative forcing, the optical properties of BCFAs are modelled. Owing to the high computational time involved in numerical modelling, there are some gaps in terms of data coverage and knowledge regarding how optical properties of coated BCFAs vary over the range of different factors (size, shape, and composition). This investigation bridged those gaps by following a state-of-the-art description scheme of BCFAs based on morphology, composition, and wavelength. The BCFA optical properties were investigated as a function of the radius of the primary particle (ao), fractal dimension (Df), fraction of organics (forganics), wavelength (λ), and mobility diameter (Dmob). The optical properties are calculated using the multiple-sphere T-matrix (MSTM) method. For the first time, the modelled optical properties of BC are expressed in terms of mobility diameter (Dmob), making the results more relevant and relatable for ambient and laboratory BC studies. Amongst size, morphology, and composition, all the optical properties showed the highest variability with changing size. The cross sections varied from 0.0001 to 0.1 µm2 for BCFA Dmob ranging from 24 to 810 nm. It has been shown that MACBC and single-scattering albedo (SSA) are sensitive to morphology, especially for larger particles with Dmob > 100 nm. Therefore, while using the simplified core–shell representation of BC in global models, the influence of morphology on radiative forcing estimations might not be adequately considered. The Ångström absorption exponent (AAE) varied from 1.06 up to 3.6 and increased with the fraction of organics (forganics). Measurement results of AAE ≫ 1 are often misinterpreted as biomass burning aerosol, it was observed that the AAE of purely black carbon particles can be ≫ 1 in the case of larger BC particles. The values of the absorption enhancement factor (Eλ) via coating were found to be between 1.01 and 3.28 in the visible spectrum. The Eλ was derived from Mie calculations for coated volume equivalent spheres and from MSTM for coated BCFAs. Mie-calculated enhancement factors were found to be larger by a factor of 1.1 to 1.5 than their corresponding values calculated from the MSTM method. It is shown that radiative forcings are highly sensitive to modifications in morphology and composition. The black carbon radiative forcing ΔFTOA (W m−2) decreases up to 61 % as the BCFA becomes more compact, indicating that global model calculations should account for changes in morphology. A decrease of more than 50 % in ΔFTOA was observed as the organic content of the particle increased up to 90 %. The changes in the ageing factors (composition and morphology) in tandem result in an overall decrease in the ΔFTOA. A parameterization scheme for optical properties of BC fractal aggregates was developed, which is applicable for modelling, ambient, and laboratory-based BC studies. The parameterization scheme for the cross sections (extinction, absorption, and scattering), single-scattering albedo (SSA), and asymmetry parameter (g) of pure and coated BCFAs as a function of Dmob were derived from tabulated results of the MSTM method. Spanning an extensive parameter space, the developed parameterization scheme showed promisingly high accuracy up to 98 % for the cross sections, 97 % for single-scattering albedos (SSAs), and 82 % for the asymmetry parameter (g).

scholarly journals Variation of the radiative properties during black carbon aging: theoretical and experimental intercomparison

2015 ◽  
Vol 15 (14) ◽  
pp. 19835-19872 ◽  
Author(s):  
C. He ◽  
K.-N. Liou ◽  
Y. Takano ◽  
R. Zhang ◽  
M. L. Zamora ◽  
...  
Keyword(s):  
Black Carbon ◽  
Cross Sections ◽  
Theoretical Calculations ◽  
Absorption Enhancement ◽  
Core Shell ◽  
Hygroscopic Growth ◽  
Aging Model ◽  
Scattering Cross ◽  
Coating Morphology ◽  
Scattering Cross Sections

Abstract. A theoretical black carbon (BC) aging model is developed to account for three typical evolution stages, namely, freshly emitted aggregates, coated BC by soluble material, and BC particles undergoing further hygroscopic growth. The geometric-optics surface-wave (GOS) approach is employed to compute the BC single-scattering properties at each aging stage, which are subsequently compared with laboratory measurements. Theoretical calculations are consistent with measurements in extinction and absorption cross sections for fresh BC aggregates, but overestimate the scattering cross sections for BC mobility diameters of 155, 245, and 320 nm, because of uncertainties associated with theoretical calculations for small particles as well as laboratory scattering measurements. The measured optical cross sections for coated BC by sulfuric acid and for those undergoing further hygroscopic growth are captured by theoretical calculations using a concentric core-shell structure, with differences of less than 20 %. This suggests that the core-shell shape represents the realistic BC coating morphology reasonably well in this case, which is consistent with the observed strong structure compaction during aging. We find that the absorption and scattering properties of fresh BC aggregates vary by up to 60 % due to uncertainty in the BC refractive index, which, however, is a factor of two smaller in the case of coated BC particles. Sensitivity analyses on the BC morphology show that the optical properties of fresh BC aggregates are more sensitive to fractal dimension than primary spherule size. The absorption and scattering cross sections of coated BC particles vary by more than a factor of two due to different coating structures. We find an increase of 20–250 % in absorption and a factor of 3–15 in scattering during aging, significantly depending on coating morphology and aging stages. Applying the aging model to CalNex 2010 field measurements, we show that the resulting BC direct radiative forcing (DRF) first increases from 1.5 to 1.7 W m-2 and subsequently decreases to 1.0 W m-2 during the transport from the Los Angeles Basin to downwind regions, as a result of the competition between absorption enhancement due to coating and dilution of BC concentration. The BC DRF can vary by up to a factor of two due to differences in BC coating morphology. Thus, an accurate estimate of BC DRF requires the incorporation of a dynamic BC aging process that accounts for realistic morphology in climate models, particularly for the regional analysis with high atmospheric heterogeneity.

Hourly concentrations and light scattering cross sections for fine particle sulfate at Big Bend National Park

2003 ◽  
Vol 37 (9-10) ◽  
pp. 1175-1183 ◽  
Author(s):  
Susanne V Hering ◽  
Mark R Stolzenburg ◽  
Jenny L Hand ◽  
Sonia M Kreidenweis ◽  
Taehyoung Lee ◽  
...  
Keyword(s):  
Light Scattering ◽  
Cross Sections ◽  
Fine Particle ◽  
National Park ◽  
Big Bend National Park ◽  
Scattering Cross ◽  
Big Bend ◽  
Scattering Cross Sections

scholarly journals Optical properties of sea ice doped with black carbon – an experimental and radiative-transfer modelling comparison

2017 ◽  
Vol 11 (6) ◽  
pp. 2867-2881 ◽  
Author(s):  
Amelia A. Marks ◽  
Maxim L. Lamare ◽  
Martin D. King
Keyword(s):  
Radiative Transfer ◽  
Sea Ice ◽  
Black Carbon ◽  
Cross Sections ◽  
Extinction Coefficient ◽  
Radiative Transfer Model ◽  
First Year ◽  
Transfer Model ◽  
Ice Fabrics ◽  
Scattering Cross Sections

Abstract. Radiative-transfer calculations of the light reflectivity and extinction coefficient in laboratory-generated sea ice doped with and without black carbon demonstrate that the radiative-transfer model TUV-snow can be used to predict the light reflectance and extinction coefficient as a function of wavelength. The sea ice is representative of first-year sea ice containing typical amounts of black carbon and other light-absorbing impurities. The experiments give confidence in the application of the model to predict albedo of other sea ice fabrics. Sea ices,  ∼  30 cm thick, were generated in the Royal Holloway Sea Ice Simulator ( ∼  2000 L tanks) with scattering cross sections measured between 0.012 and 0.032 m2 kg−1 for four ices. Sea ices were generated with and without  ∼  5 cm upper layers containing particulate black carbon. Nadir reflectances between 0.60 and 0.78 were measured along with extinction coefficients of 0.1 to 0.03 cm−1 (e-folding depths of 10–30 cm) at a wavelength of 500 nm. Values were measured between light wavelengths of 350 and 650 nm. The sea ices generated in the Royal Holloway Sea Ice Simulator were found to be representative of natural sea ices. Particulate black carbon at mass ratios of  ∼  75,  ∼  150 and  ∼  300 ng g−1 in a 5 cm ice layer lowers the albedo to 97, 90 and 79 % of the reflectivity of an undoped clean sea ice (at a wavelength of 500 nm).

scholarly journals Variation of the radiative properties during black carbon aging: theoretical and experimental intercomparison

2015 ◽  
Vol 15 (20) ◽  
pp. 11967-11980 ◽  
Author(s):  
C. He ◽  
K.-N. Liou ◽  
Y. Takano ◽  
R. Zhang ◽  
M. Levy Zamora ◽  
...  
Keyword(s):  
Black Carbon ◽  
Cross Sections ◽  
Climate Models ◽  
Theoretical Calculations ◽  
Accurate Estimate ◽  
Radiative Properties ◽  
Sensitivity Analyses ◽  
Hygroscopic Growth ◽  
Scattering Cross ◽  
Scattering Cross Sections

Abstract. A theoretical black carbon (BC) aging model is developed to account for three typical evolution stages, namely, freshly emitted aggregates, BC coated by soluble material, and BC particles undergoing further hygroscopic growth. The geometric-optics surface-wave (GOS) approach is employed to compute the BC single-scattering properties at each aging stage, which are subsequently compared with laboratory measurements. Theoretical calculations are consistent with measurements in extinction and absorption cross sections for fresh BC aggregates with different BC sizes (i.e., mobility diameters of 155, 245, and 320 nm), with differences of ≤ 25 %. The measured optical cross sections for BC coated by sulfuric acid and for that undergoing further hygroscopic growth are generally captured (differences < 30 %) by theoretical calculations using a concentric core-shell structure, with an overestimate in extinction and absorption of the smallest BC size and an underestimate in scattering of the largest BC size. We find that the absorption and scattering cross sections of fresh BC aggregates vary by 20–40 and 50–65 %, respectively, due to the use of upper (1.95–0.79i) and lower (1.75–0.63i) bounds of BC refractive index, while the variations are < 20 % in absorption and < 50 % in scattering in the case of coated BC particles. Sensitivity analyses of the BC morphology show that the optical properties of fresh BC aggregates are more sensitive to fractal dimension than primary spherule size. The absorption and scattering cross sections of coated BC particles vary by more than a factor of 2 due to different coating structures. We find an increase of 20–250 % in absorption and a factor of 3–15 in scattering during aging, significantly depending on coating morphology and aging stages. This study suggests that an accurate estimate of BC radiative effects requires the incorporation of a dynamic BC aging process that accounts for realistic coating structures in climate models.

scholarly journals Black carbon aerosol number and mass concentration measurements by picosecond short-range elastic backscatter lidar

2021 ◽  
Author(s):  
Romain Ceolato ◽  
Andres Bedoya-Velasquez ◽  
Frederic Fossard ◽  
Vincent Mouysset ◽  
Lucas Paulien ◽  
...  
Keyword(s):  
Black Carbon ◽  
Cross Sections ◽  
Time Resolution ◽  
Mass Concentration ◽  
Short Range ◽  
Small Scale ◽  
Inversion Method ◽  
Remote Measurement ◽  
Fractal Aggregates ◽  
Black Carbon Aerosol

Abstract Black carbon aerosol emissions are recognized as contributors to global warming and air pollution. There remains, however, a lack of in-situ techniques to remotely quantify black carbon aerosol particles with high range and time resolution. This article presents for the first time, to our knowledge, a direct and contact-free remote measurement of black carbon aerosol number and mass concentration less than ten of meters from the emission source. This is done with a novel picosecond short-range elastic backscatter lidar (PSR-EBL) technique. To address the complexity of retrieving lidar products at short measurement ranges, we apply a forward inversion method featuring radiometric lidar calibration. Our method is based on an extension of a well-established light-scattering model, the Rayleigh-Debye-Gans for Fractal-Aggregates (RDG-FA) theory, which computes an analytical expression for lidar parameters. These parameters are the backscattering cross-sections and the lidar ratio for black carbon fractal aggregates. Using a small-scale Jet A-1 kerosene pool fire, it is shown that our technique can quantify the aerosol number and mass concentration with centimetre range-resolution and millisecond time-resolution.

scholarly journals Radiative properties of coated black carbon aggregates: numerical simulations and radiative forcing estimates

2021 ◽  
Author(s):  
Baseerat Romshoo ◽  
Thomas Müller ◽  
Sascha Pfeifer ◽  
Jorge Saturno ◽  
Andreas Nowak ◽  
...  
Keyword(s):  
Black Carbon ◽  
Cross Section ◽  
Cross Sections ◽  
Asymmetry Parameter ◽  
Radiative Forcing ◽  
Single Scattering ◽  
Radiative Properties ◽  
Absorption Cross ◽  
Parametrization Scheme ◽  
The Cross

Abstract. The formation of black carbon fractal aggregates (BCFAs) from combustion and subsequent aging involves several stages resulting in modifications of particle size, morphology, and composition over time. To understand and quantify how each of these modifications influences the BC radiative forcing, the radiative properties of BCFAs are modelled. Owing to the high computational time involved in numerical modelling, there are some gaps in terms of data coverage and knowledge regarding how radiative properties of coated BCFAs vary over the range of different factors (size, shape, and composition). This investigation bridged those gaps by following a state-of-the-art description scheme of BCFAs based on morphology, composition, and wavelength. The BCFAs radiative properties were investigated as a function of the radius of the primary particle (ao), fractal dimension (Df), fraction of organics (forganics), wavelength (λ), and mobility diameter (Dmob). The radiative properties are calculated using the multiple sphere T-matrix (MSTM) method. Amongst size, morphology, and composition, all the radiative properties showed the highest variability with changing size. The cross-sections varied from 0.0001 μm2 to 0.1 μm2 for BCFA Dmob ranging from 24 nm to 810 nm. After size or Dmob, the absorption cross-section (Cabs) and BC mass absorption cross-section (MACBC) showed the highest sensitivity towards composition or forganics, whereas the asymmetry parameter (g) showed higher dependence on morphology, which is represented by Df. The Ångstrom absorption exponent varied from 1.06 up to 3.6 and increases with the fraction of organics (forganics). The values of the absorption enhancement factor (Eλ) were found between 1.01 and 3.28 in the visible spectrum. The Eλ was derived from Mie calculations for coated volume equivalent spheres, and from MSTM for coated BCFAs. Mie calculated enhancement factors were found to be larger by a factor of 1.1 to 1.5 than their corresponding values calculated from the MSTM method. It is shown that radiative forcings are highly sensitive towards modifications in morphology and composition. The black carbon radiative forcing ΔFTOA (Wm−2) decreases up to 61 % as the BCFA becomes more compact in morphology. Whereas, there is a decrease of > 50 % in ΔFTOA as the organic content of the particle increase up to 90 %. Based on our results, which showed a significant effect of coating and morphology on the BC radiative properties, a parametrization scheme for radiative properties of BC fractal aggregates was developed, which is applicable for modelling, ambient, and laboratory-based BC studies. The parameterization scheme for the cross-sections (extinction, absorption, and scattering), single scattering albedo (SSA), and asymmetry parameter (g) of pure and coated BCFAs as a function of Dmob were derived from tabulated results of the MSTM method. Spanning over an extensive parameter space, the developed parametrization scheme showed promisingly high accuracy up to 98 % for the cross-sections, 97 % for single scattering albedos (SSA), and 82 % for asymmetry parameter (g).

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