Abstract

Light absorbing carbon aerosols play a substantial role in climate change through radiative forcing, which is the dominant absorber of solar radiation. Radiative properties of light absorbing carbon aerosols are strongly dependent on the morphological factors and the mixing mechanism of black carbon with other aerosol components. This study focuses on the morphological effects on the optical properties of internally mixed light absorbing carbon aerosols using the numerically exact superposition T-matrix method. Three types aerosols with different aging status such as freshly emitted BC particles, thinly coated light absorbing carbon aerosols, heavily coated light absorbing carbon aerosols are studied. Our study showed that morphological factors change with the aging of internally mixed light absorbing carbon aerosols to result in a dramatic change in their optical properties. The absorption properties of light absorbing carbon aerosols can be enhanced approximately a factor of 2 at 0.67 um, and these enhancements depend on the morphological factors. A larger shell/core diameter ratio of volume-equivalent shell-core spheres (S/C), which indicates the degree of coating, leads to stronger absorption. The enhancement of absorption properties accompanies a greater enhancement of scattering properties, which is reflected in an increase in single scattering albedo (SSA). The enhancement of single scattering albedo due to the morphological effects can reach a factor of 3.75 at 0.67 μm. The asymmetry parameter has a similar yet smaller enhancement. Moreover, the corresponding optical properties of shell-and-core model determined by using Lorenz -Mie solutions are presented for comparison. We found that the optical properties of internally mixed light absorbing carbon aerosol can differ fundamentally from those calculated for the Mie theory shell-and-core model, particularly for thinly coated light absorbing carbon aerosols. Our studies indicate that the complex morphology of internally mixed light absorbing carbon aerosols must be explicitly considered in climate radiation balance.

© 2014 Optical Society of America

1. Introduction

Light absorbing carbon aerosols affects Earth’s energy budget by absorbing solar radiation, influencing cloud processes, and altering the melting of snow and ice cover [1, 2]. Due to the black carbon (BC) that dominates absorption of visible solar radiation, light absorbing carbon aerosols could be the one of the most important anthropogenic components of global warming after CO2 in terms of direct forcing [2]. Thus, detailed knowledge of the radiative properties of light absorbing carbon aerosols is needed to clarify the mechanisms of aerosol radiative forcing [3, 4]. Thus far, however, the uncertainties in net climate forcing from light absorbing carbon aerosols are substantial [5, 6].

BC in light absorbing carbon aerosols, which is co-emitted with a variety of other aerosols and aerosol precursor gases, has a complex, fractal-like aggregate structure [7]. Soon after emission, BC mixes with other aerosol components in the atmosphere [8, 9] which can strongly influence the balance of radiative forcing by light absorbing carbon aerosols [10, 11]. The absorption of light absorbing carbon aerosols can be significantly enhanced by internal mixing with other aerosols [1214]. However, on the basis in situ measurement studies on urban plumes, the radiative absorption enhancement for internal mixed light absorbing carbon aerosols may have been overestimated in models [1517]. The determination of and accounting for the BC mixing state with other aerosol species is very complex and has not been completely resolved thus far.

The effects of BC morphology on the optical properties of light absorbing carbon aerosols with the external mixing state have been widely studied, and have been determined to have a strong influence on the radiative properties of externally mixed light absorbing carbon aerosols [1821]. However, by far the most wide-spread method for computing the optical properties of internally mixed light absorbing carbon aerosols is to approximate aerosols by homogeneous spheres, with the assumption that BC is uniformly coated by a concentric shell of weakly absorbent material [22, 23]. The morphology of internally mixed light absorbing carbon aerosols is very complex, depending on the degree of aging, ambient temperature, and relative humidity [24, 25]. Because the morphological effects on the radiative properties of internally mixed light absorbing carbon aerosols have not been completely resolved, additional sophisticated optical models need to be employed for computing the optical properties of such aerosols with different morphological properties.

To investigate and quantify the morphological effects on the radiative properties of internally mixed light absorbing carbon aerosols and their effects on climate, it is essential to adequately model the entire complexity of the interrelationship of optical, physical, and chemical aerosol properties. Remarkable progress in modeling of light scattering by complex fractal aggregate particles has been achieved during the last two decades. The discrete dipole approximation (DDA) method has been used to calculate the optical properties of light absorbing carbon aggregates mixed with other aerosol [7, 25, 26]. In order to improve efficiency of DDA method, simple alternatives models, such as the “core-grey-shell” model [27], are studied to particularly fast compute the optical properties of internally mixed light absorbing carbon aerosols. Moreover, recent theory developments of the superposition T-matrix method enable calculation of the optical properties of internally mixed light absorbing carbon aerosols with various morphologies [28, 29]. The radiative properties of these aerosols can be accurate calculated by using the Multiple Sphere T-Matrix model [30, 31]. The scattering and absorption properties of micrometer-sized water droplets contaminated by black carbon were calculated using extended superposition T-matrix [32].

The aim of this study is to investigate the radiative properties of internally mixed light absorbing carbon aerosols by comprehensively and quantitatively evaluating the morphological effects on the optical properties of light absorbing carbon aerosols. The findings should improve our understanding of the morphological effects on the radiative properties of internally mixed light absorbing carbon aerosols and their effects on climate.

2. Methodology

2.1 Internally mixed light absorbing carbon aerosol models with various morphological properties

Results of in situ measurements and laboratory studies indicate that freshly emitted BC particles tends to be coated with a thin layer of other aerosol components in the atmosphere through the coagulation and condensation of secondary aerosol compounds [3335]. With the aging of the light absorbing carbon particles, most BC particles are thickly coated and tend to be compact [36, 37]. The irregular geometry and complex microstructure of light absorbing carbon agglomerates have been suggested to enhance the condensation of organic and inorganic components because of decreased equilibrium vapor pressure from the negative curvature (Kelvin) effect, particularly for larger particles [38, 39].

The aging process of light absorbing carbon aerosols results in a dramatic change in morphological parameters. Freshly emitted BC particles consist of small spherical primary particles combined into branched aggregates (Fig. 1(a)). For thinly coated light absorbing carbon aerosols, the BC particles are thinly coated by other aerosol components, and the morphology of the BC particles is still visible (Fig. 1(b)). For heavily coated light absorbing carbon aerosols, however, the BC particles are embedded into other aerosol components, and the morphology of BC particles is not visible (Fig. 1(c)).

 

Fig. 1 Transmission electron microscope images of (a) freshly emitted black carbon (BC) particles [40], (b) thinly coated light absorbing carbon aerosols [41], and (c) heavily coated light absorbing carbon aerosols [26].

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The morphologies of freshly emitted BC particles, thinly coated light absorbing carbon aerosols, and heavily coated light absorbing carbon aerosols can be modeled by using the parallel diffusion limited aggregation (DLA) algorithm [42]. The construction and morphology of the fractal clusters can be described by the well-known statistical scaling law. In this way, the relationship of the number of the monomer in a cluster Ns and the radius of gyration Rgcan be linked by the fractal prefactor k0and the fractal dimensionDf. The specific types of clusters were simulated by using the parallel DLA algorithm with input parameters such asNs, k0,Df.

Compared with freshly BC particles (Fig. 2(a)), each monomer of thinly coated light absorbing carbon aerosols can be assumed as having structures of a concentric core containing BC particles with high absorption and a shell containing weakly absorbing particles, such as organic (Fig. 2(b)) rather than the spherical homogeneous simplification. For heavily coated light absorbing carbon aerosols, BC particles are engulfed in the other components. In such cases, the morphology alters to compact closed structures, and the morphology of other materials coated on the BC particles is simply assumed as homogeneous spheres (Fig. 2(c)). The other material coating the BC particles is assumed to be sulfate in this study. The morphological properties of internally mixed light absorbing carbon aerosols [4346] are shown in Table 1.The S/C ratio of the soot-sulfate mixtures are defined as the diameter ratio of the volume-equivalent spherical soot core without sulfate shell and the total volume-equivalent sphere with sulfate shell.

 

Fig. 2 Schematic diagram showing the transformation of light absorbing carbon aggregates with increasing mass fraction of condensed materials: (a) freshly emitted black carbon (BC) particles, (b) thinly coated light absorbing carbon aerosols, (c) heavily coated light absorbing carbon aerosols.

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Tables Icon

Table 1. Morphological Properties of Internally Mixed Light Absorbing Carbon Aerosols

The refractive indices of BC particles are those reported by Change and Charalampopulos [47], whereas the refractive indices of sulfate were obtained from the Optical Properties of Aerosols and Clouds (OPAC) database [48].

2.2 Superposition T-matrix method

The superposition T-matrix approach, which uses the numerically exact solution methods to Maxwell’s equations, can be used to calculate the T-matrix descriptions of the light scattering from the cluster with an appropriate superposition technique, and analytically obtain the random-orientation cross sections and scattering matrices of these clusters. Until now, the superposition solution for scattering by a system of optically active spheres is extended to the case where any of the spheres can be located at points that are either internal or external to the other sphere [30].

Using the parallel diffusion limited aggregation (DLA) algorithm and the morphological features in field-emission transmission electron microscope images, the construction and morphology of internally mixed light absorbing carbon aerosols are modeled to initialize the superposition T-matrix model, MSTM version 3.0 programs. The absorption, scattering and extinction efficiencies are the output variables of the MSTM program.

In the open-source Fortran coded MSTM version 3.0 program, both exteral and internal mixtures are applicable with the only limitation that the spherical surfaces are nonoverlapping. Each spherical surface will have an associated host sphere, which being the sphere whose refractive index is in contact with the exterior surface. The external medium of these scatters is assumed as vacuum. The random orientation scattering properties are obtained analytically from the superposition T-matrix model method, and can be averaged by multiple calculations for different clusters with the same morphological parameters.

3. Optical properties of internally mixed light absorbing carbon aerosols with various morphological properties

The absorption cross sections of light absorbing carbon aerosols represent one of the major factors leading to large uncertainties in the evaluation of light absorbing carbon aerosol climate effects. Figure 3 shows the variation of absorption cross sections of internally mixed light absorbing carbon aerosols with various morphological parameters, including freshly emitted BC particles, thinly coated light absorbing carbon aerosols, and heavily coated light absorbing carbon aerosols. The mass absorption cross sections (MAC) can be computed from the absorption cross sections, which are defined as the absorption cross sections per unit mass of light absorbing carbon.

 

Fig. 3 Absorption cross sections (Cabs) of internally mixed light absorbing carbon aerosols with various morphological factors: freshly emitted BC particles (Df = 2.0, S/C = 1.0), thinly coated light absorbing carbon aerosols (Df = 2.4, S/C = 1.5), and heavily coated light absorbing carbon aerosols (Df = 2.8, S/C = 2.0).

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Estimated of MAC depend on the assumed refractive index and mass density of BC particles. Bond and Bergstrom [49] recommend the values of refractive index at 0.55 μm as following values: m=1.75+0.63i, m=1.80+0.67i, m=1.85+0.71i, m=1.90+0.75i, and m=1.95+0.79i. The density of real BC particles recommended as 1.7-1.9g/cm3 [49]. We assume the refractive indexm=1.75+0.63i, and the densityρBC=1.8g/cm3. For freshly emitted BC particles, the estimated MAC value (at 0.55 μm) is 5.5m2/g. When the refractive index ism=1.95+0.79i, the estimated MAC value (at 0.55 μm) is 6.03m2/g. Estimated of MAC are in agreement with the range of theoretical modeled values [50, 51] and smaller than the values modeled by Scarnato et al. [52] using a discrete dipole approximation model. Estimated of MAC lies in the range of field measurements of MAC for carbonaceous particles varying from 5 to 25m2/g [53, 54], although these values lie below the range ofMAC=(7.5±1.2)m2/g recommended by Bond and Bergstrom [49] based on the publications of measurements.

During the alternation of these morphological parameters, the light absorption can be enhanced approximately a factor of 2, where the enhancement is defined asCabscoated/Cabsfresh, at 0.67 um, and the enhancements depend on the morphological parameters. The coating increases the geometric cross section of the particles, thus intercepting more electromagnetic energy, which, inside the particle, interacts with the highly absorbing carbonaceous material, thus increasing the absorption cross section. For thinly coated light absorbing carbon aerosols, the enhancement is approximately a factor of 1.1 at 0.67 um; that for heavily coated light absorbing carbon aerosols can reach a factor of 2.

Figure 4 shows the variation of scattering properties including single scattering albedo and asymmetry parameter of internally mixed light absorbing carbon aerosols with various morphological parameters. For freshly emitted BC particles, the single scattering albedo was as low as 0.20 at 0.67um, which is consistent with the measurements for fresh diesel exhaust light absorbing carbon [55], and in agreement with the suggested value of0.25±0.05 (at 0.55 μm) [49]. The mass extinction cross sections (MEC) can be retrieved from the mass absorption cross sections and single scattering albedo. When the refractive index ism=1.95+0.79iand the density isρBC=1.8g/cm3, the estimated MEC value (at 0.633 μm) is 7.4m2/g, which lie below in the range of MEC=(8.7±1.1)m2/g recommended by Mulholland and Croarkin [56] based on the publications of measurements. Possible sources of bias are the choices of refractive index and the density of BC particles.

 

Fig. 4 Single scattering albedo (SSA) and asymmetry parameter (ASY) of internally mixed light absorbing carbon aerosols with various morphological factors: freshly emitted black carbon particles (Df = 2.0, S/C = 1.0), thinly coated light absorbing carbon aerosols (Df = 2.4, S/C = 1.5), and heavily coated light absorbing carbon aerosols (Df = 2.8, S/C = 2.0).

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The scattering properties of coated light absorbing carbon aerosols were significantly higher than those of freshly emitted black carbon particles, even for thinly coated light absorbing carbon aerosols. The single scattering albedo changed from 0.2 for freshly emitted BC particles to 0.4 for thinly coated light absorbing carbon up to 0.75 for heavily coated light absorbing carbon. Moreover, the asymmetry parameter changed from 0.45 for freshly emitted BC particles to 0.7 for heavily coated light absorbing carbon.

During the aging process of light absorbing carbon aerosols, the enhancement of absorption properties accompany an enhancement of scattering properties, which is reflected by an increase in single scattering albedo. The asymmetry parameter also increased during the aging process, which indicates that there is less scattering of incoming radiation back to its source. The enhanced single scattering albedo and asymmetry parameter can lead to a decrease in solar radiation absorption into the atmospheric layer [5759].

4. Effects of morphology on the optical properties of internally mixed aerosols

During the aging process of light absorbing carbon aerosols, optical properties such as absorption and scattering are dramatically changed due to the effects of morphology such as formation of coated shell and compaction of BC particles. To quantitatively evaluate the morphological effects on the optical properties of light absorbing carbon aerosols, the shell/core ratio (S/C) was used to represent the states of coating, and fractal dimensions were used to represent the states of compaction of the BC particles.

4.1. Effects of shell/core ratio (S/C)

The S/C is an important factor in the enhancement of optical properties of internally mixed light absorbing carbon aerosols. Figure 5 shows the variation of absorption cross sections of internally mixed light absorbing carbon aerosols with different shell/core ratio (S/C). During the aging process, a larger S/C leads to stronger absorption. The absorption was enlarged from 0.05 (S/C = 1.1) to 0.1 (S/C = 2.0) at 0.67 μm, which corresponds to an enhancement of a factor of 2. Decreasing the size parameter (x=πD/λ, where Dis the particle diameter and λis the wavelength) resulted in an increase in absorption enhancement. For thinly coated light absorbing carbon, the enhancement of absorption properties due to S/C reached to a factor of 1.25 at 0.44 μm, whereas the enhancement at 1.02 μm can be ignored. For heavily coated light absorbing carbon, the enhancement of absorption properties due to S/C reached a factor of 1.27 at 0.44 μm, whereas the enhancement at 1.02 μm reached a factor of 1.2.

 

Fig. 5 Absorption cross sections of internally mixed light absorbing carbon aerosols with various shell/core ratio (S/C): (a) thinly coated light absorbing carbon aerosol (Df = 2.4, S/C = 1.1, 1.3, 1.5), (b) heavily coated light absorbing carbon aerosol (Df = 2.8, S/C = 1.5, 1.75, 2.0).

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Coating BC particles with sulfate resulted in dramatic changes in scattering properties (Figs. 6 and 7). During the aging process, a larger S/C leads to stronger scattering properties (single scattering albedo and asymmetry parameter). The single scattering albedo was enlarged from 0.25 (S/C = 1.1) to 0.72 (S/C = 2.0) at 0.67 μm, which corresponds to an enhancement of a factor of 2.88. The asymmetry parameter was enlarged from 0.6 (S/C = 1.1) to 0.7 (S/C = 2.0) at 0.67 μm, which corresponds to an enhancement of a factor of 1.17. For thinly coated light absorbing carbon, the enhancement of single scattering albedo due to S/C reached a factor of 1.68 at 0.67 μm, whereas for heavily coated light absorbing carbon, the value reached a factor of 1.38 at 0.67 μm. The asymmetry parameter had a similar yet smaller enhancement.

 

Fig. 6 Single scattering albedo (SSA) and asymmetry parameter (ASY) of thinly coated light absorbing carbon aerosols with various shell/core ratio (S/C). Df = 2.4, S/C = 1.1, 1.3, 1.5.

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Fig. 7 Single scattering albedo (SSA) and asymmetry parameter (ASY) of heavily coated light absorbing carbon aerosols with various shell/core ratio (S/C). Df = 2.8, S/C = 1.5, 1.75, 2.0.

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4.2. Effects of fractal dimensions

The effects of Df on the optical properties of freshly emitted BC particles were studied, and results indicate Dfis a very important morphological parameter for the evaluation of the optical properties of such particles. In this study, therefore, the effects of Df on the optical properties of only thinly coated light absorbing carbon aerosols and heavily coated light absorbing carbon aerosols were studied.

Figure 8 shows the variation of absorption cross sections of internally mixed light absorbing carbon aerosols (thinly coated and heavily coated) with various fractal dimensions (Df). Contrary to effects of Dfon the absorption cross sections of freshly emitted BC particles, for thinly coated aerosol, the effects of Df on the absorption cross sections can be ignored. This general behavior was also found by Wu et al. [31]. Figures 9 and 10 show the effects of fractal dimensions on the scattering properties of internally mixed light absorbing carbon aerosols. For thinly coated light absorbing carbon aerosols, values of single scattering albedo are higher for compact aggregates than for lacy aggregates, due to a stronger scattering interaction and stronger electromagnetic coupling between spherules [60]. The effects of fractal dimensions enhanced various in single scattering albedo and the asymmetry parameter a factor of 1.18 and 1.10 at 0.67 μm. For heavily coated light absorbing carbon aerosols, the effects of fractal dimensions on the scattering properties were small and can be ignored due to the effect of sulfate in the heavy coating.

 

Fig. 8 Absorption cross sections of internally mixed light absorbing carbon aerosols with various fractal dimensions (Df): (a) thinly coated light absorbing carbon aerosol (Df = 2.2, 2.4, 2.6, S/C = 1.5), (b) heavily coated light absorbing carbon aerosol (Df = 2.6, 2.8, 3.0, S/C = 1.75).

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Fig. 9 Single scattering albedo (SSA) and asymmetry parameter (ASY) of thinly coated light absorbing carbon aerosols with various fractal dimensions (Df = 2.2, 2.4, 2.6, S/C = 1.5)

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Fig. 10 Single scattering albedo (SSA) and asymmetry parameter (ASY) of heavily coated light absorbing carbon aerosols with various fractal dimensions (Df = 2.6, 2.8, 3.0, S/C = 1.75)

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5. Optical properties of alteration of internally mixed light absorbing carbon aerosols due to assumption of concentric spherical core–shell model

Thus far, the most wide-spread method used for computing the optical properties of internally mixed light absorbing carbon aerosols is the Mie theory with a shell-and-core model, which approximates BC particles by homogeneous spheres with the assumption that BC is uniformly coated by a concentric shell of weakly absorbent material. To quantify the morphological effects on the radiative properties of internally mixed light absorbing carbon aerosols and their effects on climate, the corresponding optical properties of the Mie theory shell-and-core model are presented for comparison.

Figures 11 and 12 show the ranges for optical properties of internally mixed light absorbing carbon aerosols (thinly coated, and heavily coated) with alteration due to assumption of the concentric spherical core-shell model. For thinly coated light absorbing carbon aerosols, the Mie theory shell-and-core model resulted in a dramatic change in the internally mixed light absorbing carbon aerosol optical properties. In this model, the variation of extinction coefficient reached 80%, and the variation of absorption properties reached 40%, where the variation is defined as(CMSTMCMei)/CMSTM100%. The scattering properties, including single scattering albedo and asymmetry parameter showed similar changes. The variation of single scattering albedo reached 60%, and the variation of asymmetry parameter reached 60%.

 

Fig. 11 Ranges for optical properties of thinly coated light absorbing carbon aerosols with alterations due to assumption of the concentric spherical core-shell model (Df = 2.4, S/C = 1.1, 1.3, 1.5).

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Fig. 12 Ranges for optical properties of heavily coated light absorbing carbon aerosols with alteration due to assumption of the concentric spherical core-shell model (Df = 2.8, S/C = 1.5, 1.75, 2.0).

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For the heavily coated light absorbing carbon aerosols the variation of extinction coefficient was smaller than 20%, and the variation of absorption properties was smaller than 10%. For scattering properties, the variation of single scattering albedo was smaller than 10%, and the variation of asymmetry parameter was smaller than 20%. Compared with thinly coated light absorbing carbon aerosols, the ranges for optical properties of heavily coated light absorbing carbon aerosols with alteration due to the assumption of the concentric spherical core-shell model were weakened.

The optical properties of internally mixed light absorbing carbon aerosol can differ fundamentally from those calculated for Mie theory shell-and-core model, particularly for thinly coated light absorbing carbon aerosol. This indicates that the complex morphology of internally mixed light absorbing carbon aerosols must be explicitly considered in climate radiation balance.

6. Summary and discussion

In this study, morphological effects on the optical properties of internally mixed light absorbing carbon aerosols with different aging status are studied using the numerically exact superposition T-matrix method. The aging process of light absorbing carbon aerosols resulted in dramatic changes in the morphological factors including coating and compaction. During the morphological parameter alteration, the light absorption was enhanced approximately a factor of 2, where the enhancement is defined asCabscoated/Cabsfresh, at 0.67 um, and the enhancements depended on the morphological factors. A larger S/C leads to stronger absorption. The absorption was enlarged from 0.05 (S/C = 1.1) to 0.1 (S/C = 2.0) at 0.67 μm, which corresponds to an enhancement of a factor of 2.

The enhancement of absorption properties accompanied greater enhancement of scattering properties larger enhanced, which was reflected in the increase in single scattering albedo. The single scattering albedo changed from 0.2 for freshly emitted BC particles to 0.4 for thinly coated light absorbing carbon up to 0.75 for heavily coated light absorbing carbon. The asymmetry parameter also increased due to the changes in morphological parameters, which indicates that there was less scattering of incoming radiation back to its source. The asymmetry parameter changed from 0.45 for freshly emitted BC particles to 0.7 for heavily coated light absorbing carbon. A larger S/C leads to stronger scattering properties (single scattering albedo and asymmetry parameter). The single scattering albedo was enlarged from 0.25 (S/C = 1.1) to 0.72 (S/C = 2.0) at 0.67 μm, which corresponds to an enhancement of a factor of 2.88. The asymmetry parameter was enlarged from 0.6 (S/C = 1.1) to 0.7 (S/C = 2.0) at 0.67 μm, which corresponds to an enhancement of a factor of 1.17. Such enhancement in single scattering albedo and the asymmetry parameter can lead to a decrease in solar radiation absorption into the atmospheric layer.

Our studies show that the optical properties of internally mixed light absorbing carbon aerosol can differ fundamentally from those calculated for the Mie theory shell-and-core model, particularly for thinly coated light absorbing carbon aerosol. For thinly coated light absorbing carbon aerosols, the Mie theory shell-and-core model resulted in the variation of extinction coefficient reached 80%, the variation of absorption properties reached 40%, the variation of single scattering albedo reached 60%, and the variation of asymmetry parameter reached 60%, where the variation is defined as(CMSTMCMei)/CMSTM100%. In order to improve the accurate shell-and-core model simulation, some simple alternatives were studied, such as the “core-grey-shell” model, which seems to give highly accurate results.

Our studies indicate that the complex morphologies of internally mixed light absorbing carbon aerosols must be explicitly considered in the climate radiation balance. These findings should improve our understanding of morphological effects on the radiative properties of internally mixed light absorbing carbon aerosols and their effects on climate.

Acknowledgments

This research was supported by the National Natural Science Foundation of China (Grant No: 41371015, 41001207), the National Basic Research Program of China (973 Program) (Grant No: 2010CB950800), the Funds of the Chinese Academy of Sciences for Key Topics in Innovation Engineering (Grant No: KZCX2-EW-QN311). We would like to acknowledge the authors of superposition T-matrix: Daniel Mackowski, Kirk Fuller, and Michael Mishchenko. The code of MSTM version 3.0 was downloaded from http://www.eng.auburn.edu/users/dmckwski/scatcodes/.

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16. C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Response to comment on “Radiative absorption enhancements due to the mixing state of atmospheric black carbon”,” Science 339(6118), 393 (2013). [CrossRef]   [PubMed]  

17. M. Z. Jacobson, “Comment on “radiative absorption enhancements due to the mixing state of atmospheric black carbon”,” Science 339(6118), 393 (2013). [CrossRef]   [PubMed]  

18. M. I. Mishchenko, L. Liu, L. D. Travis, and A. A. Lacis, “Scattering and radiative properties of semi-external versus external mixtures of different aerosol types,” J. Quant. Spectrosc. Radiat. Transfer 88(1–3), 139–147 (2004). [CrossRef]  

19. M. Kahnert, “Modelling the optical and radiative properties of freshly emitted light absorbing carbon within an atmospheric chemical transport model,” Atmos. Chem. Phys. 10(3), 1403–1416 (2010). [CrossRef]  

20. L. Liu and M. I. Mishchenko, “Effects of aggregation on scattering and radiative properties of soot aerosols,” J. Geophys. Res. 110, D11211 (2005). [CrossRef]  

21. T. Cheng, X. Gu, Y. Wu, H. Chen, and T. Yu, “The optical properties of absorbing aerosols with fractal soot aggregates: Implications for aerosol remote sensing,” J. Quant. Spectrosc. Radiat. Transfer 125, 93–104 (2013).

22. T. P. Ackerman and O. B. Toon, “Absorption of visible radiation in atmosphere containing mixtures of absorbing and nonabsorbing particles,” Appl. Opt. 20(20), 3661–3667 (1981). [CrossRef]   [PubMed]  

23. J. P. Schwarz, J. R. Spackman, D. W. Fahey, R. S. Gao, U. Lohmann, P. Stier, L. A. Watts, D. S. Thomson, D. A. Lack, L. Pfister, M. J. Mahoney, D. Baumgardner, J. C. Wilson, and J. M. Reeves, “Coatings and their enhancement of black carbon light absorption in the tropical atmosphere,” J. Geophys. Res. 113, D03203 (2008).

24. J. Li, M. Pósfai, P. V. Hobbs, and P. R. Buseck, “Individual aerosol particles from biomass burning in southern Africa: 2. Compositions and aging of inorganic particles,” J. Geophys. Res. 108, 8484 (2003).

25. M. Kahnert, T. Nousiainen, H. Lindqvist, and M. Ebert, “Optical properties of light absorbing carbon aggregates mixed with sulfate: assessment of different model geometries for climate forcing calculations,” Opt. Express 20(9), 10042–10058 (2012). [CrossRef]   [PubMed]  

26. A. Worringen, M. Ebert, T. Trautmann, S. Weinbruch, and G. Helas, “Optical properties of internally mixed ammonium sulfate and soot particles--a study of individual aerosol particles and ambient aerosol populations,” Appl. Opt. 47(21), 3835–3845 (2008). [CrossRef]   [PubMed]  

27. M. Kahnert, T. Nousiainen, and H. Lindqvist, “Models for integrated and differential scattering optical properties of encapsulated light absorbing carbon aggregates,” Opt. Express 21(7), 7974–7993 (2013). [CrossRef]   [PubMed]  

28. D. W. Mackowski and M. I. Mishchenko, “A multiple sphere T-matrix Fortran code for use on parallel computer clusters,” J. Quant. Spectrosc. Radiat. Transfer 112(13), 2182–2192 (2011). [CrossRef]  

29. M. I. Mishchenko, G. Videen, N. G. Khlebtsov, and T. Wriedt, “Comprehensive T-matrix reference database: A 2012–2013 update,” J. Quant. Spectrosc. Radiat. Transfer 123, 145–152 (2013). [CrossRef]  

30. D. W. Mackowski, “A general superposition solution for electromagnetic scattering by multiple spherical domains of optically active media,” J. Quant. Spectrosc. Radiat. Transfer 133, 264–270 (2014). [CrossRef]  

31. Y. Wu, T. Cheng, X. Gu, L. Zheng, H. Chen, and H. Xu, “The single scattering properties of soot aggregates with concentric core–shell spherical monomers,” J. Quant. Spectrosc. Radiat. Transfer 135, 9–19 (2014). [CrossRef]  

32. M. I. Mishchenko, L. Liu, B. Cairns, and D. W. Mackowski, “Optics of water cloud droplets mixed with black-carbon aerosols,” Opt. Lett. 39(9), 2607–2610 (2014). [CrossRef]   [PubMed]  

33. T. Tritscher, Z. Jurányi, M. Martin, R. Chirico, M. Gysel, M. F. Heringa, P. F. DeCarlo, B. Sierau, A. S. H. Prévôt, E. Weingartner, and U. Baltensperger, “Changes of hygroscopicity and morphology during ageing of diesel soot,” Environ. Res. Lett. 6, 034026 (2011). [CrossRef]  

34. J. P. Schwarz, R. S. Gao, J. R. Spackman, L. A. Watts, D. S. Thomson, D. W. Fahey, T. B. Ryerson, J. Peischl, J. S. Holloway, M. Trainer, G. J. Frost, T. Baynard, D. A. Lack, J. A. de Gouw, C. Warneke, and L. A. Del Negro, “Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions,” Geophys. Res. Lett. 35(13), L13810 (2008). [CrossRef]  

35. S. China, C. Mazzoleni, K. Gorkowski, A. C. Aiken, and M. K. Dubey, “Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles,” Nat. Commun. 4, 2122 (2013). [CrossRef]   [PubMed]  

36. E. Coz and C. Leck, “Morphology and state of mixture of atmospheric soot aggregates during the winter season over Southern Asia–a quantitative approach,” Tellus Ser. B 63, 107–116 (2011). [CrossRef]  

37. R. Zhang, A. F. Khalizov, J. Pagels, D. Zhang, H. Xue, and P. H. McMurry, “Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing,” Proc. Natl. Acad. Sci. U. S. A. 105, 10291–10296 (2008). [CrossRef]  

38. A. F. Khalizov, R. Zhang, D. Zhang, H. Xue, J. Pagels, and P. H. McMurry, “Formation of highly hygroscopic light absorbing carbon aerosols upon internal mixing with sulfuric acid vapor,” J. Geophys. Res. 114, D05208 (2009).

39. Y. Crouzet and W. H. Marlow, “Calculations of the equilibrium vapor pressure of water over adhering 50–200-nm spheres,” Aerosol Sci. Technol. 22(1), 43–59 (1995). [CrossRef]  

40. M. Wentzel, H. Gorzawski, K. H. Naumann, H. Saathoff, and S. Weinbruch, “Transmission electron microscopical and aerosol dynamical characterization of soot aerosols,” J. Aerosol Sci. 34(10), 1347–1370 (2003). [CrossRef]  

41. P. R. Buseck, K. Adachi, A. Gelencsér, É. Tompa, and M. Po’sfai, “Are black carbon and soot the same?” Atmos. Chem. Phys. Discuss. 12, 24821–24846 (2012).

42. H. G. E. Hentschel, “Fractal dimension of generalized diffusion-limited aggregates,” Phys. Rev. Lett. 52(3), 212–215 (1984). [CrossRef]  

43. J. Hallett, J. G. Hudson, and C. F. Rogers, “Characterization of combustion aerosols for haze and cloud formation,” Aerosol Sci. Technol. 10(1), 70–83 (1989). [CrossRef]  

44. G. Ramachandran and P. C. Reist, “Characterization of morphological changes in agglomerates subject to condensation and evaporation using multiple fractal dimensions,” Aerosol Sci. Technol. 23(3), 431–442 (1995). [CrossRef]  

45. S. Nyeki and I. Colbeck, “Fractal dimension analysis of single, in-situ, restructured carbonaceous aggregates,” Aerosol Sci. Technol. 23(2), 109–120 (1995). [CrossRef]  

46. C. M. Sorensen and G. C. Roberts, “The prefactor of fractal aggregates,” J. Colloid Interface Sci. 186(2), 447–452 (1997). [CrossRef]   [PubMed]  

47. H. Chang and T. T. Charalampopoulos, “Determination of the wavelength dependence of refractive indices of flame soot,” Proc. R. Soc. London A Math. Phys. Sci. 430, 577–591 (1990). [CrossRef]  

48. M. Hess, P. Koepke, and I. Schult, “Optical properties of aerosols and clouds: The software package OPAC,” Bull. Am. Meteorol. Soc 79(5), 831–844 (1998). [CrossRef]  

49. T. C. Bond and R. W. Bergstrom, “Light absorption by carbonaceous particles: An investigative review,” Aerosol Sci. Technol. 40(1), 27–67 (2006). [CrossRef]  

50. M. Kahnert, “On the discrepancy between modeled and measured mass absorption cross sections of light absorbing carbon aerosols,” Aerosol Sci. Technol. 44(6), 453–460 (2010). [CrossRef]  

51. M. Kahnert, “Numerically exact computation of the optical properties of light absorbing carbon aggregates for wavelength of 200 nm–12.2 μm,” Atmos. Chem. Phys. 10(17), 8319–8329 (2010). [CrossRef]  

52. B. V. Scarnato, S. Vahidinia, D. T. Richard, and T. W. Kirchstetter, “Effects of internal mixing and aggregate morphology on optical properties of black carbon using a discrete dipole approximation model,” Atmos. Chem. Phys. 13(10), 5089–5101 (2013). [CrossRef]  

53. B. J. Huebert, T. Bates, P. B. Russell, G. Shi, Y. J. Kim, K. Kawamura, G. Carmichael, and T. Nakajima, “An overview of ACE‐Asia: Strategies for quantifying the relationships between Asian aerosols and their climatic impacts,” J. Geophys. Res. 108, 8633 (2003).

54. P. K. Quinn, D. J. Coffman, T. S. Bates, E. J. Welton, D. S. Covert, T. L. Miller, J. E. Johnson, S. Maria, L. Russell, R. Arimoto, C. M. Carrico, M. J. Rood, and J. Anderson, “Aerosol optical properties measured on board the Ronald H. Brown during ACE-Asia as a function of aerosol chemical composition and source region,” J. Geophys. Res. 109(D19), D19S01 (2004). [CrossRef]  

55. M. Schnaiter, H. Horvath, O. Möhler, K. H. Naumann, H. Saathoff, and O. W. Schöck, “UV-VIS-NIR spectral optical properties of soot and soot-containing aerosols,” J. Aerosol Sci. 34(10), 1421–1444 (2003). [CrossRef]  

56. G. W. Mulholland and C. Croarkin, “Specific extinction coefficient of flame generated smoke,” Fire Mater. 24(5), 227–230 (2000). [CrossRef]  

57. Y. Takemura, T. Nakajima, O. Dubovik, B. N. Holben, and S. Kinne, “Single-scattering albedo and radiative forcing of various aerosol species with a global three-dimensional model,” J. Clim. 15(4), 333–352 (2002). [CrossRef]  

58. R. W. Bergstrom, P. B. Russell, and P. Hignett, “Wavelength dependence of the absorption of black carbon particles: Predictions and results from the TARFOX experiment and implications for the aerosol single scattering albedo,” J. Atmos. Sci. 59(3), 567–577 (2002). [CrossRef]  

59. M. Fiebig and J. A. Ogren, “Retrieval and climatology of the aerosol asymmetry parameter in the NOAA aerosol monitoring network,” J. Geophys. Res. 111, D21204 (2006).

60. L. Liu, M. I. Mishchenko, and W. P. Arnott, “A study of radiative properties of fractal soot aggregates using the superposition T-matrix method,” J. Quant. Spectrosc. Radiat. Transfer 109(15), 2656–2663 (2008). [CrossRef]  

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  29. M. I. Mishchenko, G. Videen, N. G. Khlebtsov, and T. Wriedt, “Comprehensive T-matrix reference database: A 2012–2013 update,” J. Quant. Spectrosc. Radiat. Transfer 123, 145–152 (2013).
    [Crossref]
  30. D. W. Mackowski, “A general superposition solution for electromagnetic scattering by multiple spherical domains of optically active media,” J. Quant. Spectrosc. Radiat. Transfer 133, 264–270 (2014).
    [Crossref]
  31. Y. Wu, T. Cheng, X. Gu, L. Zheng, H. Chen, and H. Xu, “The single scattering properties of soot aggregates with concentric core–shell spherical monomers,” J. Quant. Spectrosc. Radiat. Transfer 135, 9–19 (2014).
    [Crossref]
  32. M. I. Mishchenko, L. Liu, B. Cairns, and D. W. Mackowski, “Optics of water cloud droplets mixed with black-carbon aerosols,” Opt. Lett. 39(9), 2607–2610 (2014).
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    [Crossref]
  35. S. China, C. Mazzoleni, K. Gorkowski, A. C. Aiken, and M. K. Dubey, “Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles,” Nat. Commun. 4, 2122 (2013).
    [Crossref] [PubMed]
  36. E. Coz and C. Leck, “Morphology and state of mixture of atmospheric soot aggregates during the winter season over Southern Asia–a quantitative approach,” Tellus Ser. B 63, 107–116 (2011).
    [Crossref]
  37. R. Zhang, A. F. Khalizov, J. Pagels, D. Zhang, H. Xue, and P. H. McMurry, “Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing,” Proc. Natl. Acad. Sci. U. S. A. 105, 10291–10296 (2008).
    [Crossref]
  38. A. F. Khalizov, R. Zhang, D. Zhang, H. Xue, J. Pagels, and P. H. McMurry, “Formation of highly hygroscopic light absorbing carbon aerosols upon internal mixing with sulfuric acid vapor,” J. Geophys. Res. 114, D05208 (2009).
  39. Y. Crouzet and W. H. Marlow, “Calculations of the equilibrium vapor pressure of water over adhering 50–200-nm spheres,” Aerosol Sci. Technol. 22(1), 43–59 (1995).
    [Crossref]
  40. M. Wentzel, H. Gorzawski, K. H. Naumann, H. Saathoff, and S. Weinbruch, “Transmission electron microscopical and aerosol dynamical characterization of soot aerosols,” J. Aerosol Sci. 34(10), 1347–1370 (2003).
    [Crossref]
  41. P. R. Buseck, K. Adachi, A. Gelencsér, É. Tompa, and M. Po’sfai, “Are black carbon and soot the same?” Atmos. Chem. Phys. Discuss. 12, 24821–24846 (2012).
  42. H. G. E. Hentschel, “Fractal dimension of generalized diffusion-limited aggregates,” Phys. Rev. Lett. 52(3), 212–215 (1984).
    [Crossref]
  43. J. Hallett, J. G. Hudson, and C. F. Rogers, “Characterization of combustion aerosols for haze and cloud formation,” Aerosol Sci. Technol. 10(1), 70–83 (1989).
    [Crossref]
  44. G. Ramachandran and P. C. Reist, “Characterization of morphological changes in agglomerates subject to condensation and evaporation using multiple fractal dimensions,” Aerosol Sci. Technol. 23(3), 431–442 (1995).
    [Crossref]
  45. S. Nyeki and I. Colbeck, “Fractal dimension analysis of single, in-situ, restructured carbonaceous aggregates,” Aerosol Sci. Technol. 23(2), 109–120 (1995).
    [Crossref]
  46. C. M. Sorensen and G. C. Roberts, “The prefactor of fractal aggregates,” J. Colloid Interface Sci. 186(2), 447–452 (1997).
    [Crossref] [PubMed]
  47. H. Chang and T. T. Charalampopoulos, “Determination of the wavelength dependence of refractive indices of flame soot,” Proc. R. Soc. London A Math. Phys. Sci. 430, 577–591 (1990).
    [Crossref]
  48. M. Hess, P. Koepke, and I. Schult, “Optical properties of aerosols and clouds: The software package OPAC,” Bull. Am. Meteorol. Soc 79(5), 831–844 (1998).
    [Crossref]
  49. T. C. Bond and R. W. Bergstrom, “Light absorption by carbonaceous particles: An investigative review,” Aerosol Sci. Technol. 40(1), 27–67 (2006).
    [Crossref]
  50. M. Kahnert, “On the discrepancy between modeled and measured mass absorption cross sections of light absorbing carbon aerosols,” Aerosol Sci. Technol. 44(6), 453–460 (2010).
    [Crossref]
  51. M. Kahnert, “Numerically exact computation of the optical properties of light absorbing carbon aggregates for wavelength of 200 nm–12.2 μm,” Atmos. Chem. Phys. 10(17), 8319–8329 (2010).
    [Crossref]
  52. B. V. Scarnato, S. Vahidinia, D. T. Richard, and T. W. Kirchstetter, “Effects of internal mixing and aggregate morphology on optical properties of black carbon using a discrete dipole approximation model,” Atmos. Chem. Phys. 13(10), 5089–5101 (2013).
    [Crossref]
  53. B. J. Huebert, T. Bates, P. B. Russell, G. Shi, Y. J. Kim, K. Kawamura, G. Carmichael, and T. Nakajima, “An overview of ACE‐Asia: Strategies for quantifying the relationships between Asian aerosols and their climatic impacts,” J. Geophys. Res. 108, 8633 (2003).
  54. P. K. Quinn, D. J. Coffman, T. S. Bates, E. J. Welton, D. S. Covert, T. L. Miller, J. E. Johnson, S. Maria, L. Russell, R. Arimoto, C. M. Carrico, M. J. Rood, and J. Anderson, “Aerosol optical properties measured on board the Ronald H. Brown during ACE-Asia as a function of aerosol chemical composition and source region,” J. Geophys. Res. 109(D19), D19S01 (2004).
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2014 (3)

D. W. Mackowski, “A general superposition solution for electromagnetic scattering by multiple spherical domains of optically active media,” J. Quant. Spectrosc. Radiat. Transfer 133, 264–270 (2014).
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Y. Wu, T. Cheng, X. Gu, L. Zheng, H. Chen, and H. Xu, “The single scattering properties of soot aggregates with concentric core–shell spherical monomers,” J. Quant. Spectrosc. Radiat. Transfer 135, 9–19 (2014).
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M. I. Mishchenko, L. Liu, B. Cairns, and D. W. Mackowski, “Optics of water cloud droplets mixed with black-carbon aerosols,” Opt. Lett. 39(9), 2607–2610 (2014).
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2013 (8)

S. China, C. Mazzoleni, K. Gorkowski, A. C. Aiken, and M. K. Dubey, “Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles,” Nat. Commun. 4, 2122 (2013).
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T. Cheng, X. Gu, Y. Wu, H. Chen, and T. Yu, “The optical properties of absorbing aerosols with fractal soot aggregates: Implications for aerosol remote sensing,” J. Quant. Spectrosc. Radiat. Transfer 125, 93–104 (2013).

M. Kahnert, T. Nousiainen, and H. Lindqvist, “Models for integrated and differential scattering optical properties of encapsulated light absorbing carbon aggregates,” Opt. Express 21(7), 7974–7993 (2013).
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T. C. Bond, S. J. Doherty, D. W. Fahey, P. M. Forster, T. Berntsen, O. Boucher, B. J. DeAngelo, M. G. Flanner, S. Ghan, B. Kärcher, D. Koch, S. Kinne, Y. Kondo, P. K. Quinn, M. C. Sarofim, M. G. Schultz, M. Schulz, C. Venkataraman, H. Zhang, S. Zhang, N. Bellouin, S. K. Guttikunda, P. K. Hopke, M. Z. Jacobson, J. W. Kaiser, Z. Klimont, U. Lohmann, J. P. Schwarz, D. Shindell, T. Storelvmo, S. G. Warren, and C. S. Zender, “Bounding the role of black carbon in the climate system: A scientific assessment,” J. Geophys. Res. Atmos. 118, 5380–5552 (2013).

C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Response to comment on “Radiative absorption enhancements due to the mixing state of atmospheric black carbon”,” Science 339(6118), 393 (2013).
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M. Z. Jacobson, “Comment on “radiative absorption enhancements due to the mixing state of atmospheric black carbon”,” Science 339(6118), 393 (2013).
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M. I. Mishchenko, G. Videen, N. G. Khlebtsov, and T. Wriedt, “Comprehensive T-matrix reference database: A 2012–2013 update,” J. Quant. Spectrosc. Radiat. Transfer 123, 145–152 (2013).
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B. V. Scarnato, S. Vahidinia, D. T. Richard, and T. W. Kirchstetter, “Effects of internal mixing and aggregate morphology on optical properties of black carbon using a discrete dipole approximation model,” Atmos. Chem. Phys. 13(10), 5089–5101 (2013).
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2012 (3)

P. R. Buseck, K. Adachi, A. Gelencsér, É. Tompa, and M. Po’sfai, “Are black carbon and soot the same?” Atmos. Chem. Phys. Discuss. 12, 24821–24846 (2012).

C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Radiative absorption enhancements due to the mixing state of atmospheric black carbon,” Science 337(6098), 1078–1081 (2012).
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M. Kahnert, T. Nousiainen, H. Lindqvist, and M. Ebert, “Optical properties of light absorbing carbon aggregates mixed with sulfate: assessment of different model geometries for climate forcing calculations,” Opt. Express 20(9), 10042–10058 (2012).
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2011 (3)

D. W. Mackowski and M. I. Mishchenko, “A multiple sphere T-matrix Fortran code for use on parallel computer clusters,” J. Quant. Spectrosc. Radiat. Transfer 112(13), 2182–2192 (2011).
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E. Coz and C. Leck, “Morphology and state of mixture of atmospheric soot aggregates during the winter season over Southern Asia–a quantitative approach,” Tellus Ser. B 63, 107–116 (2011).
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T. Tritscher, Z. Jurányi, M. Martin, R. Chirico, M. Gysel, M. F. Heringa, P. F. DeCarlo, B. Sierau, A. S. H. Prévôt, E. Weingartner, and U. Baltensperger, “Changes of hygroscopicity and morphology during ageing of diesel soot,” Environ. Res. Lett. 6, 034026 (2011).
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2010 (4)

M. Kahnert, “Modelling the optical and radiative properties of freshly emitted light absorbing carbon within an atmospheric chemical transport model,” Atmos. Chem. Phys. 10(3), 1403–1416 (2010).
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K. Adachi, S. H. Chung, and P. R. Buseck, “Shapes of light absorbing carbon aerosol particles and implications for their effects on climate,” J. Geophys. Res. 115, D15206 (2010).

M. Kahnert, “On the discrepancy between modeled and measured mass absorption cross sections of light absorbing carbon aerosols,” Aerosol Sci. Technol. 44(6), 453–460 (2010).
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M. Kahnert, “Numerically exact computation of the optical properties of light absorbing carbon aggregates for wavelength of 200 nm–12.2 μm,” Atmos. Chem. Phys. 10(17), 8319–8329 (2010).
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2009 (2)

A. F. Khalizov, H. Xue, L. Wang, J. Zheng, and R. Zhang, “Enhanced light absorption and scattering by carbon soot aerosol internally mixed with sulfuric acid,” J. Phys. Chem. A 113, 1066–1074 (2009).
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2008 (7)

R. Zhang, A. F. Khalizov, J. Pagels, D. Zhang, H. Xue, and P. H. McMurry, “Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing,” Proc. Natl. Acad. Sci. U. S. A. 105, 10291–10296 (2008).
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J. P. Schwarz, R. S. Gao, J. R. Spackman, L. A. Watts, D. S. Thomson, D. W. Fahey, T. B. Ryerson, J. Peischl, J. S. Holloway, M. Trainer, G. J. Frost, T. Baynard, D. A. Lack, J. A. de Gouw, C. Warneke, and L. A. Del Negro, “Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions,” Geophys. Res. Lett. 35(13), L13810 (2008).
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A. Worringen, M. Ebert, T. Trautmann, S. Weinbruch, and G. Helas, “Optical properties of internally mixed ammonium sulfate and soot particles--a study of individual aerosol particles and ambient aerosol populations,” Appl. Opt. 47(21), 3835–3845 (2008).
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J. P. Schwarz, J. R. Spackman, D. W. Fahey, R. S. Gao, U. Lohmann, P. Stier, L. A. Watts, D. S. Thomson, D. A. Lack, L. Pfister, M. J. Mahoney, D. Baumgardner, J. C. Wilson, and J. M. Reeves, “Coatings and their enhancement of black carbon light absorption in the tropical atmosphere,” J. Geophys. Res. 113, D03203 (2008).

V. Ramanathan and G. Carmichael, “Global and regional climate changes due to black carbon,” Nat. Geosci. 1(4), 221–227 (2008).
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K. Adachi and P. R. Buseck, “Internally mixed soot, sulfates, and organic matter in aerosol particles from Mexico City,” Atmos. Chem. Phys. 8, 6469–6481 (2008).
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L. Liu, M. I. Mishchenko, and W. P. Arnott, “A study of radiative properties of fractal soot aggregates using the superposition T-matrix method,” J. Quant. Spectrosc. Radiat. Transfer 109(15), 2656–2663 (2008).
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2007 (1)

N. Moteki and Y. Kondo, “Effects of mixing state on black carbon measurements by laser-induced incandescence,” Aerosol Sci. Technol. 41(4), 398–417 (2007).
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2006 (3)

T. C. Bond, G. Habib, and R. W. Bergstrom, “Limitations in the enhancement of visible light absorption due to mixing state,” J. Geophys. Res. 111, D20211 (2006).

T. C. Bond and R. W. Bergstrom, “Light absorption by carbonaceous particles: An investigative review,” Aerosol Sci. Technol. 40(1), 27–67 (2006).
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M. Fiebig and J. A. Ogren, “Retrieval and climatology of the aerosol asymmetry parameter in the NOAA aerosol monitoring network,” J. Geophys. Res. 111, D21204 (2006).

2005 (4)

N. Bellouin, O. Boucher, J. Haywood, and M. S. Reddy, “Global estimate of aerosol direct radiative forcing from satellite measurements,” Nature 438(7071), 1138–1141 (2005).
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K. S. Johnson, B. Zuberi, L. T. Molina, M. J. Molina, M. J. Iedema, J. P. Cowin, D. J. Gaspar, C. Wang, and A. Laskin, “Processing of soot in an urban environment: case study from the Mexico City Metropolitan Area,” Atmos. Chem. Phys. 5, 3033–3043 (2005).
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M. Schnaiter, C. Linke, O. Möhler, K.-H. Naumann, H. Saathoff, R. Wagner, U. Schurath, and B. Wehner, “Absorption amplification of black carbon internally mixed with secondary organic aerosol,” J. Geophys. Res. 110, D19204 (2005).

L. Liu and M. I. Mishchenko, “Effects of aggregation on scattering and radiative properties of soot aerosols,” J. Geophys. Res. 110, D11211 (2005).
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2004 (2)

M. I. Mishchenko, L. Liu, L. D. Travis, and A. A. Lacis, “Scattering and radiative properties of semi-external versus external mixtures of different aerosol types,” J. Quant. Spectrosc. Radiat. Transfer 88(1–3), 139–147 (2004).
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P. K. Quinn, D. J. Coffman, T. S. Bates, E. J. Welton, D. S. Covert, T. L. Miller, J. E. Johnson, S. Maria, L. Russell, R. Arimoto, C. M. Carrico, M. J. Rood, and J. Anderson, “Aerosol optical properties measured on board the Ronald H. Brown during ACE-Asia as a function of aerosol chemical composition and source region,” J. Geophys. Res. 109(D19), D19S01 (2004).
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2003 (4)

M. Schnaiter, H. Horvath, O. Möhler, K. H. Naumann, H. Saathoff, and O. W. Schöck, “UV-VIS-NIR spectral optical properties of soot and soot-containing aerosols,” J. Aerosol Sci. 34(10), 1421–1444 (2003).
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B. J. Huebert, T. Bates, P. B. Russell, G. Shi, Y. J. Kim, K. Kawamura, G. Carmichael, and T. Nakajima, “An overview of ACE‐Asia: Strategies for quantifying the relationships between Asian aerosols and their climatic impacts,” J. Geophys. Res. 108, 8633 (2003).

M. Wentzel, H. Gorzawski, K. H. Naumann, H. Saathoff, and S. Weinbruch, “Transmission electron microscopical and aerosol dynamical characterization of soot aerosols,” J. Aerosol Sci. 34(10), 1347–1370 (2003).
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J. Li, M. Pósfai, P. V. Hobbs, and P. R. Buseck, “Individual aerosol particles from biomass burning in southern Africa: 2. Compositions and aging of inorganic particles,” J. Geophys. Res. 108, 8484 (2003).

2002 (3)

S. H. Chung and J. H. Seinfeld, “Global distribution and climate forcing of carbonaceous aerosols,” J. Geophys. Res. 107(D19), 4407 (2002).

Y. Takemura, T. Nakajima, O. Dubovik, B. N. Holben, and S. Kinne, “Single-scattering albedo and radiative forcing of various aerosol species with a global three-dimensional model,” J. Clim. 15(4), 333–352 (2002).
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R. W. Bergstrom, P. B. Russell, and P. Hignett, “Wavelength dependence of the absorption of black carbon particles: Predictions and results from the TARFOX experiment and implications for the aerosol single scattering albedo,” J. Atmos. Sci. 59(3), 567–577 (2002).
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2001 (2)

V. Ramanathan, P. J. Crutzen, J. Lelieveld, A. P. Mitra, D. Althausen, J. Anderson, M. O. Andreae, W. Cantrell, G. R. Cass, C. E. Chung, A. D. Clarke, J. A. Coakley, W. D. Collins, W. C. Conant, F. Dulac, J. Heintzenberg, A. J. Heymsfield, B. Holben, S. Howell, J. Hudson, A. Jayaraman, J. T. Kiehl, T. N. Krishnamurti, D. Lubin, G. McFarquhar, T. Novakov, J. A. Ogren, I. A. Podgorny, K. Prather, K. Priestley, J. M. Prospero, P. K. Quinn, K. Rajeev, P. Rasch, S. Rupert, R. Sadourny, S. K. Satheesh, G. E. Shaw, P. Sheridan, and F. P. J. Valero, “Indian Ocean Experiment: An integrated analysis of the climate forcing and effects of the great Indo-Asian haze,” J. Geophys. Res. 106(D22), 28371–28398 (2001).
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M. Z. Jacobson, “Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols,” Nature 409(6821), 695–697 (2001).
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2000 (1)

G. W. Mulholland and C. Croarkin, “Specific extinction coefficient of flame generated smoke,” Fire Mater. 24(5), 227–230 (2000).
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1998 (1)

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C. M. Sorensen and G. C. Roberts, “The prefactor of fractal aggregates,” J. Colloid Interface Sci. 186(2), 447–452 (1997).
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G. Ramachandran and P. C. Reist, “Characterization of morphological changes in agglomerates subject to condensation and evaporation using multiple fractal dimensions,” Aerosol Sci. Technol. 23(3), 431–442 (1995).
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H. Chang and T. T. Charalampopoulos, “Determination of the wavelength dependence of refractive indices of flame soot,” Proc. R. Soc. London A Math. Phys. Sci. 430, 577–591 (1990).
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J. Hallett, J. G. Hudson, and C. F. Rogers, “Characterization of combustion aerosols for haze and cloud formation,” Aerosol Sci. Technol. 10(1), 70–83 (1989).
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H. G. E. Hentschel, “Fractal dimension of generalized diffusion-limited aggregates,” Phys. Rev. Lett. 52(3), 212–215 (1984).
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Ackerman, T. P.

Adachi, K.

P. R. Buseck, K. Adachi, A. Gelencsér, É. Tompa, and M. Po’sfai, “Are black carbon and soot the same?” Atmos. Chem. Phys. Discuss. 12, 24821–24846 (2012).

K. Adachi, S. H. Chung, and P. R. Buseck, “Shapes of light absorbing carbon aerosol particles and implications for their effects on climate,” J. Geophys. Res. 115, D15206 (2010).

K. Adachi and P. R. Buseck, “Internally mixed soot, sulfates, and organic matter in aerosol particles from Mexico City,” Atmos. Chem. Phys. 8, 6469–6481 (2008).
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Aiken, A. C.

S. China, C. Mazzoleni, K. Gorkowski, A. C. Aiken, and M. K. Dubey, “Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles,” Nat. Commun. 4, 2122 (2013).
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Althausen, D.

V. Ramanathan, P. J. Crutzen, J. Lelieveld, A. P. Mitra, D. Althausen, J. Anderson, M. O. Andreae, W. Cantrell, G. R. Cass, C. E. Chung, A. D. Clarke, J. A. Coakley, W. D. Collins, W. C. Conant, F. Dulac, J. Heintzenberg, A. J. Heymsfield, B. Holben, S. Howell, J. Hudson, A. Jayaraman, J. T. Kiehl, T. N. Krishnamurti, D. Lubin, G. McFarquhar, T. Novakov, J. A. Ogren, I. A. Podgorny, K. Prather, K. Priestley, J. M. Prospero, P. K. Quinn, K. Rajeev, P. Rasch, S. Rupert, R. Sadourny, S. K. Satheesh, G. E. Shaw, P. Sheridan, and F. P. J. Valero, “Indian Ocean Experiment: An integrated analysis of the climate forcing and effects of the great Indo-Asian haze,” J. Geophys. Res. 106(D22), 28371–28398 (2001).
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Anderson, J.

P. K. Quinn, D. J. Coffman, T. S. Bates, E. J. Welton, D. S. Covert, T. L. Miller, J. E. Johnson, S. Maria, L. Russell, R. Arimoto, C. M. Carrico, M. J. Rood, and J. Anderson, “Aerosol optical properties measured on board the Ronald H. Brown during ACE-Asia as a function of aerosol chemical composition and source region,” J. Geophys. Res. 109(D19), D19S01 (2004).
[Crossref]

V. Ramanathan, P. J. Crutzen, J. Lelieveld, A. P. Mitra, D. Althausen, J. Anderson, M. O. Andreae, W. Cantrell, G. R. Cass, C. E. Chung, A. D. Clarke, J. A. Coakley, W. D. Collins, W. C. Conant, F. Dulac, J. Heintzenberg, A. J. Heymsfield, B. Holben, S. Howell, J. Hudson, A. Jayaraman, J. T. Kiehl, T. N. Krishnamurti, D. Lubin, G. McFarquhar, T. Novakov, J. A. Ogren, I. A. Podgorny, K. Prather, K. Priestley, J. M. Prospero, P. K. Quinn, K. Rajeev, P. Rasch, S. Rupert, R. Sadourny, S. K. Satheesh, G. E. Shaw, P. Sheridan, and F. P. J. Valero, “Indian Ocean Experiment: An integrated analysis of the climate forcing and effects of the great Indo-Asian haze,” J. Geophys. Res. 106(D22), 28371–28398 (2001).
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Andreae, M. O.

V. Ramanathan, P. J. Crutzen, J. Lelieveld, A. P. Mitra, D. Althausen, J. Anderson, M. O. Andreae, W. Cantrell, G. R. Cass, C. E. Chung, A. D. Clarke, J. A. Coakley, W. D. Collins, W. C. Conant, F. Dulac, J. Heintzenberg, A. J. Heymsfield, B. Holben, S. Howell, J. Hudson, A. Jayaraman, J. T. Kiehl, T. N. Krishnamurti, D. Lubin, G. McFarquhar, T. Novakov, J. A. Ogren, I. A. Podgorny, K. Prather, K. Priestley, J. M. Prospero, P. K. Quinn, K. Rajeev, P. Rasch, S. Rupert, R. Sadourny, S. K. Satheesh, G. E. Shaw, P. Sheridan, and F. P. J. Valero, “Indian Ocean Experiment: An integrated analysis of the climate forcing and effects of the great Indo-Asian haze,” J. Geophys. Res. 106(D22), 28371–28398 (2001).
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Arimoto, R.

P. K. Quinn, D. J. Coffman, T. S. Bates, E. J. Welton, D. S. Covert, T. L. Miller, J. E. Johnson, S. Maria, L. Russell, R. Arimoto, C. M. Carrico, M. J. Rood, and J. Anderson, “Aerosol optical properties measured on board the Ronald H. Brown during ACE-Asia as a function of aerosol chemical composition and source region,” J. Geophys. Res. 109(D19), D19S01 (2004).
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Arnott, W. P.

L. Liu, M. I. Mishchenko, and W. P. Arnott, “A study of radiative properties of fractal soot aggregates using the superposition T-matrix method,” J. Quant. Spectrosc. Radiat. Transfer 109(15), 2656–2663 (2008).
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Baltensperger, U.

T. Tritscher, Z. Jurányi, M. Martin, R. Chirico, M. Gysel, M. F. Heringa, P. F. DeCarlo, B. Sierau, A. S. H. Prévôt, E. Weingartner, and U. Baltensperger, “Changes of hygroscopicity and morphology during ageing of diesel soot,” Environ. Res. Lett. 6, 034026 (2011).
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Bates, T.

B. J. Huebert, T. Bates, P. B. Russell, G. Shi, Y. J. Kim, K. Kawamura, G. Carmichael, and T. Nakajima, “An overview of ACE‐Asia: Strategies for quantifying the relationships between Asian aerosols and their climatic impacts,” J. Geophys. Res. 108, 8633 (2003).

Bates, T. S.

C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Response to comment on “Radiative absorption enhancements due to the mixing state of atmospheric black carbon”,” Science 339(6118), 393 (2013).
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C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Radiative absorption enhancements due to the mixing state of atmospheric black carbon,” Science 337(6098), 1078–1081 (2012).
[Crossref] [PubMed]

P. K. Quinn, D. J. Coffman, T. S. Bates, E. J. Welton, D. S. Covert, T. L. Miller, J. E. Johnson, S. Maria, L. Russell, R. Arimoto, C. M. Carrico, M. J. Rood, and J. Anderson, “Aerosol optical properties measured on board the Ronald H. Brown during ACE-Asia as a function of aerosol chemical composition and source region,” J. Geophys. Res. 109(D19), D19S01 (2004).
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Baumgardner, D.

J. P. Schwarz, J. R. Spackman, D. W. Fahey, R. S. Gao, U. Lohmann, P. Stier, L. A. Watts, D. S. Thomson, D. A. Lack, L. Pfister, M. J. Mahoney, D. Baumgardner, J. C. Wilson, and J. M. Reeves, “Coatings and their enhancement of black carbon light absorption in the tropical atmosphere,” J. Geophys. Res. 113, D03203 (2008).

Baynard, T.

J. P. Schwarz, R. S. Gao, J. R. Spackman, L. A. Watts, D. S. Thomson, D. W. Fahey, T. B. Ryerson, J. Peischl, J. S. Holloway, M. Trainer, G. J. Frost, T. Baynard, D. A. Lack, J. A. de Gouw, C. Warneke, and L. A. Del Negro, “Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions,” Geophys. Res. Lett. 35(13), L13810 (2008).
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T. C. Bond, S. J. Doherty, D. W. Fahey, P. M. Forster, T. Berntsen, O. Boucher, B. J. DeAngelo, M. G. Flanner, S. Ghan, B. Kärcher, D. Koch, S. Kinne, Y. Kondo, P. K. Quinn, M. C. Sarofim, M. G. Schultz, M. Schulz, C. Venkataraman, H. Zhang, S. Zhang, N. Bellouin, S. K. Guttikunda, P. K. Hopke, M. Z. Jacobson, J. W. Kaiser, Z. Klimont, U. Lohmann, J. P. Schwarz, D. Shindell, T. Storelvmo, S. G. Warren, and C. S. Zender, “Bounding the role of black carbon in the climate system: A scientific assessment,” J. Geophys. Res. Atmos. 118, 5380–5552 (2013).

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J. P. Schwarz, R. S. Gao, J. R. Spackman, L. A. Watts, D. S. Thomson, D. W. Fahey, T. B. Ryerson, J. Peischl, J. S. Holloway, M. Trainer, G. J. Frost, T. Baynard, D. A. Lack, J. A. de Gouw, C. Warneke, and L. A. Del Negro, “Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions,” Geophys. Res. Lett. 35(13), L13810 (2008).
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J. P. Schwarz, J. R. Spackman, D. W. Fahey, R. S. Gao, U. Lohmann, P. Stier, L. A. Watts, D. S. Thomson, D. A. Lack, L. Pfister, M. J. Mahoney, D. Baumgardner, J. C. Wilson, and J. M. Reeves, “Coatings and their enhancement of black carbon light absorption in the tropical atmosphere,” J. Geophys. Res. 113, D03203 (2008).

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T. C. Bond, S. J. Doherty, D. W. Fahey, P. M. Forster, T. Berntsen, O. Boucher, B. J. DeAngelo, M. G. Flanner, S. Ghan, B. Kärcher, D. Koch, S. Kinne, Y. Kondo, P. K. Quinn, M. C. Sarofim, M. G. Schultz, M. Schulz, C. Venkataraman, H. Zhang, S. Zhang, N. Bellouin, S. K. Guttikunda, P. K. Hopke, M. Z. Jacobson, J. W. Kaiser, Z. Klimont, U. Lohmann, J. P. Schwarz, D. Shindell, T. Storelvmo, S. G. Warren, and C. S. Zender, “Bounding the role of black carbon in the climate system: A scientific assessment,” J. Geophys. Res. Atmos. 118, 5380–5552 (2013).

Subramanian, R.

C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Response to comment on “Radiative absorption enhancements due to the mixing state of atmospheric black carbon”,” Science 339(6118), 393 (2013).
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C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Radiative absorption enhancements due to the mixing state of atmospheric black carbon,” Science 337(6098), 1078–1081 (2012).
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Takemura, Y.

Y. Takemura, T. Nakajima, O. Dubovik, B. N. Holben, and S. Kinne, “Single-scattering albedo and radiative forcing of various aerosol species with a global three-dimensional model,” J. Clim. 15(4), 333–352 (2002).
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J. P. Schwarz, J. R. Spackman, D. W. Fahey, R. S. Gao, U. Lohmann, P. Stier, L. A. Watts, D. S. Thomson, D. A. Lack, L. Pfister, M. J. Mahoney, D. Baumgardner, J. C. Wilson, and J. M. Reeves, “Coatings and their enhancement of black carbon light absorption in the tropical atmosphere,” J. Geophys. Res. 113, D03203 (2008).

J. P. Schwarz, R. S. Gao, J. R. Spackman, L. A. Watts, D. S. Thomson, D. W. Fahey, T. B. Ryerson, J. Peischl, J. S. Holloway, M. Trainer, G. J. Frost, T. Baynard, D. A. Lack, J. A. de Gouw, C. Warneke, and L. A. Del Negro, “Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions,” Geophys. Res. Lett. 35(13), L13810 (2008).
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Tompa, É.

P. R. Buseck, K. Adachi, A. Gelencsér, É. Tompa, and M. Po’sfai, “Are black carbon and soot the same?” Atmos. Chem. Phys. Discuss. 12, 24821–24846 (2012).

Toon, O. B.

Trainer, M.

J. P. Schwarz, R. S. Gao, J. R. Spackman, L. A. Watts, D. S. Thomson, D. W. Fahey, T. B. Ryerson, J. Peischl, J. S. Holloway, M. Trainer, G. J. Frost, T. Baynard, D. A. Lack, J. A. de Gouw, C. Warneke, and L. A. Del Negro, “Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions,” Geophys. Res. Lett. 35(13), L13810 (2008).
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Trautmann, T.

Travis, L. D.

M. I. Mishchenko, L. Liu, L. D. Travis, and A. A. Lacis, “Scattering and radiative properties of semi-external versus external mixtures of different aerosol types,” J. Quant. Spectrosc. Radiat. Transfer 88(1–3), 139–147 (2004).
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T. Tritscher, Z. Jurányi, M. Martin, R. Chirico, M. Gysel, M. F. Heringa, P. F. DeCarlo, B. Sierau, A. S. H. Prévôt, E. Weingartner, and U. Baltensperger, “Changes of hygroscopicity and morphology during ageing of diesel soot,” Environ. Res. Lett. 6, 034026 (2011).
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Vahidinia, S.

B. V. Scarnato, S. Vahidinia, D. T. Richard, and T. W. Kirchstetter, “Effects of internal mixing and aggregate morphology on optical properties of black carbon using a discrete dipole approximation model,” Atmos. Chem. Phys. 13(10), 5089–5101 (2013).
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T. C. Bond, S. J. Doherty, D. W. Fahey, P. M. Forster, T. Berntsen, O. Boucher, B. J. DeAngelo, M. G. Flanner, S. Ghan, B. Kärcher, D. Koch, S. Kinne, Y. Kondo, P. K. Quinn, M. C. Sarofim, M. G. Schultz, M. Schulz, C. Venkataraman, H. Zhang, S. Zhang, N. Bellouin, S. K. Guttikunda, P. K. Hopke, M. Z. Jacobson, J. W. Kaiser, Z. Klimont, U. Lohmann, J. P. Schwarz, D. Shindell, T. Storelvmo, S. G. Warren, and C. S. Zender, “Bounding the role of black carbon in the climate system: A scientific assessment,” J. Geophys. Res. Atmos. 118, 5380–5552 (2013).

Videen, G.

M. I. Mishchenko, G. Videen, N. G. Khlebtsov, and T. Wriedt, “Comprehensive T-matrix reference database: A 2012–2013 update,” J. Quant. Spectrosc. Radiat. Transfer 123, 145–152 (2013).
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Wagner, R.

M. Schnaiter, C. Linke, O. Möhler, K.-H. Naumann, H. Saathoff, R. Wagner, U. Schurath, and B. Wehner, “Absorption amplification of black carbon internally mixed with secondary organic aerosol,” J. Geophys. Res. 110, D19204 (2005).

Wang, C.

K. S. Johnson, B. Zuberi, L. T. Molina, M. J. Molina, M. J. Iedema, J. P. Cowin, D. J. Gaspar, C. Wang, and A. Laskin, “Processing of soot in an urban environment: case study from the Mexico City Metropolitan Area,” Atmos. Chem. Phys. 5, 3033–3043 (2005).
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Wang, L.

A. F. Khalizov, H. Xue, L. Wang, J. Zheng, and R. Zhang, “Enhanced light absorption and scattering by carbon soot aerosol internally mixed with sulfuric acid,” J. Phys. Chem. A 113, 1066–1074 (2009).
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Warneke, C.

J. P. Schwarz, R. S. Gao, J. R. Spackman, L. A. Watts, D. S. Thomson, D. W. Fahey, T. B. Ryerson, J. Peischl, J. S. Holloway, M. Trainer, G. J. Frost, T. Baynard, D. A. Lack, J. A. de Gouw, C. Warneke, and L. A. Del Negro, “Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions,” Geophys. Res. Lett. 35(13), L13810 (2008).
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Warren, S. G.

T. C. Bond, S. J. Doherty, D. W. Fahey, P. M. Forster, T. Berntsen, O. Boucher, B. J. DeAngelo, M. G. Flanner, S. Ghan, B. Kärcher, D. Koch, S. Kinne, Y. Kondo, P. K. Quinn, M. C. Sarofim, M. G. Schultz, M. Schulz, C. Venkataraman, H. Zhang, S. Zhang, N. Bellouin, S. K. Guttikunda, P. K. Hopke, M. Z. Jacobson, J. W. Kaiser, Z. Klimont, U. Lohmann, J. P. Schwarz, D. Shindell, T. Storelvmo, S. G. Warren, and C. S. Zender, “Bounding the role of black carbon in the climate system: A scientific assessment,” J. Geophys. Res. Atmos. 118, 5380–5552 (2013).

Watts, L. A.

J. P. Schwarz, R. S. Gao, J. R. Spackman, L. A. Watts, D. S. Thomson, D. W. Fahey, T. B. Ryerson, J. Peischl, J. S. Holloway, M. Trainer, G. J. Frost, T. Baynard, D. A. Lack, J. A. de Gouw, C. Warneke, and L. A. Del Negro, “Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions,” Geophys. Res. Lett. 35(13), L13810 (2008).
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J. P. Schwarz, J. R. Spackman, D. W. Fahey, R. S. Gao, U. Lohmann, P. Stier, L. A. Watts, D. S. Thomson, D. A. Lack, L. Pfister, M. J. Mahoney, D. Baumgardner, J. C. Wilson, and J. M. Reeves, “Coatings and their enhancement of black carbon light absorption in the tropical atmosphere,” J. Geophys. Res. 113, D03203 (2008).

Wehner, B.

M. Schnaiter, C. Linke, O. Möhler, K.-H. Naumann, H. Saathoff, R. Wagner, U. Schurath, and B. Wehner, “Absorption amplification of black carbon internally mixed with secondary organic aerosol,” J. Geophys. Res. 110, D19204 (2005).

Weinbruch, S.

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Weingartner, E.

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Williams, E. J.

C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Response to comment on “Radiative absorption enhancements due to the mixing state of atmospheric black carbon”,” Science 339(6118), 393 (2013).
[Crossref] [PubMed]

C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Radiative absorption enhancements due to the mixing state of atmospheric black carbon,” Science 337(6098), 1078–1081 (2012).
[Crossref] [PubMed]

Wilson, J. C.

J. P. Schwarz, J. R. Spackman, D. W. Fahey, R. S. Gao, U. Lohmann, P. Stier, L. A. Watts, D. S. Thomson, D. A. Lack, L. Pfister, M. J. Mahoney, D. Baumgardner, J. C. Wilson, and J. M. Reeves, “Coatings and their enhancement of black carbon light absorption in the tropical atmosphere,” J. Geophys. Res. 113, D03203 (2008).

Worringen, A.

Worsnop, D. R.

C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Response to comment on “Radiative absorption enhancements due to the mixing state of atmospheric black carbon”,” Science 339(6118), 393 (2013).
[Crossref] [PubMed]

C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Radiative absorption enhancements due to the mixing state of atmospheric black carbon,” Science 337(6098), 1078–1081 (2012).
[Crossref] [PubMed]

Wriedt, T.

M. I. Mishchenko, G. Videen, N. G. Khlebtsov, and T. Wriedt, “Comprehensive T-matrix reference database: A 2012–2013 update,” J. Quant. Spectrosc. Radiat. Transfer 123, 145–152 (2013).
[Crossref]

Wu, Y.

Y. Wu, T. Cheng, X. Gu, L. Zheng, H. Chen, and H. Xu, “The single scattering properties of soot aggregates with concentric core–shell spherical monomers,” J. Quant. Spectrosc. Radiat. Transfer 135, 9–19 (2014).
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T. Cheng, X. Gu, Y. Wu, H. Chen, and T. Yu, “The optical properties of absorbing aerosols with fractal soot aggregates: Implications for aerosol remote sensing,” J. Quant. Spectrosc. Radiat. Transfer 125, 93–104 (2013).

Xu, H.

Y. Wu, T. Cheng, X. Gu, L. Zheng, H. Chen, and H. Xu, “The single scattering properties of soot aggregates with concentric core–shell spherical monomers,” J. Quant. Spectrosc. Radiat. Transfer 135, 9–19 (2014).
[Crossref]

Xue, H.

A. F. Khalizov, R. Zhang, D. Zhang, H. Xue, J. Pagels, and P. H. McMurry, “Formation of highly hygroscopic light absorbing carbon aerosols upon internal mixing with sulfuric acid vapor,” J. Geophys. Res. 114, D05208 (2009).

A. F. Khalizov, H. Xue, L. Wang, J. Zheng, and R. Zhang, “Enhanced light absorption and scattering by carbon soot aerosol internally mixed with sulfuric acid,” J. Phys. Chem. A 113, 1066–1074 (2009).
[Crossref] [PubMed]

R. Zhang, A. F. Khalizov, J. Pagels, D. Zhang, H. Xue, and P. H. McMurry, “Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing,” Proc. Natl. Acad. Sci. U. S. A. 105, 10291–10296 (2008).
[Crossref]

Yu, T.

T. Cheng, X. Gu, Y. Wu, H. Chen, and T. Yu, “The optical properties of absorbing aerosols with fractal soot aggregates: Implications for aerosol remote sensing,” J. Quant. Spectrosc. Radiat. Transfer 125, 93–104 (2013).

Zaveri, R. A.

C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Response to comment on “Radiative absorption enhancements due to the mixing state of atmospheric black carbon”,” Science 339(6118), 393 (2013).
[Crossref] [PubMed]

C. D. Cappa, T. B. Onasch, P. Massoli, D. R. Worsnop, T. S. Bates, E. S. Cross, P. Davidovits, J. Hakala, K. L. Hayden, B. T. Jobson, K. R. Kolesar, D. A. Lack, B. M. Lerner, S.-M. Li, D. Mellon, I. Nuaaman, J. S. Olfert, T. Petäjä, P. K. Quinn, C. Song, R. Subramanian, E. J. Williams, and R. A. Zaveri, “Radiative absorption enhancements due to the mixing state of atmospheric black carbon,” Science 337(6098), 1078–1081 (2012).
[Crossref] [PubMed]

Zender, C. S.

T. C. Bond, S. J. Doherty, D. W. Fahey, P. M. Forster, T. Berntsen, O. Boucher, B. J. DeAngelo, M. G. Flanner, S. Ghan, B. Kärcher, D. Koch, S. Kinne, Y. Kondo, P. K. Quinn, M. C. Sarofim, M. G. Schultz, M. Schulz, C. Venkataraman, H. Zhang, S. Zhang, N. Bellouin, S. K. Guttikunda, P. K. Hopke, M. Z. Jacobson, J. W. Kaiser, Z. Klimont, U. Lohmann, J. P. Schwarz, D. Shindell, T. Storelvmo, S. G. Warren, and C. S. Zender, “Bounding the role of black carbon in the climate system: A scientific assessment,” J. Geophys. Res. Atmos. 118, 5380–5552 (2013).

Zhang, D.

A. F. Khalizov, R. Zhang, D. Zhang, H. Xue, J. Pagels, and P. H. McMurry, “Formation of highly hygroscopic light absorbing carbon aerosols upon internal mixing with sulfuric acid vapor,” J. Geophys. Res. 114, D05208 (2009).

R. Zhang, A. F. Khalizov, J. Pagels, D. Zhang, H. Xue, and P. H. McMurry, “Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing,” Proc. Natl. Acad. Sci. U. S. A. 105, 10291–10296 (2008).
[Crossref]

Zhang, H.

T. C. Bond, S. J. Doherty, D. W. Fahey, P. M. Forster, T. Berntsen, O. Boucher, B. J. DeAngelo, M. G. Flanner, S. Ghan, B. Kärcher, D. Koch, S. Kinne, Y. Kondo, P. K. Quinn, M. C. Sarofim, M. G. Schultz, M. Schulz, C. Venkataraman, H. Zhang, S. Zhang, N. Bellouin, S. K. Guttikunda, P. K. Hopke, M. Z. Jacobson, J. W. Kaiser, Z. Klimont, U. Lohmann, J. P. Schwarz, D. Shindell, T. Storelvmo, S. G. Warren, and C. S. Zender, “Bounding the role of black carbon in the climate system: A scientific assessment,” J. Geophys. Res. Atmos. 118, 5380–5552 (2013).

Zhang, R.

A. F. Khalizov, H. Xue, L. Wang, J. Zheng, and R. Zhang, “Enhanced light absorption and scattering by carbon soot aerosol internally mixed with sulfuric acid,” J. Phys. Chem. A 113, 1066–1074 (2009).
[Crossref] [PubMed]

A. F. Khalizov, R. Zhang, D. Zhang, H. Xue, J. Pagels, and P. H. McMurry, “Formation of highly hygroscopic light absorbing carbon aerosols upon internal mixing with sulfuric acid vapor,” J. Geophys. Res. 114, D05208 (2009).

R. Zhang, A. F. Khalizov, J. Pagels, D. Zhang, H. Xue, and P. H. McMurry, “Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing,” Proc. Natl. Acad. Sci. U. S. A. 105, 10291–10296 (2008).
[Crossref]

Zhang, S.

T. C. Bond, S. J. Doherty, D. W. Fahey, P. M. Forster, T. Berntsen, O. Boucher, B. J. DeAngelo, M. G. Flanner, S. Ghan, B. Kärcher, D. Koch, S. Kinne, Y. Kondo, P. K. Quinn, M. C. Sarofim, M. G. Schultz, M. Schulz, C. Venkataraman, H. Zhang, S. Zhang, N. Bellouin, S. K. Guttikunda, P. K. Hopke, M. Z. Jacobson, J. W. Kaiser, Z. Klimont, U. Lohmann, J. P. Schwarz, D. Shindell, T. Storelvmo, S. G. Warren, and C. S. Zender, “Bounding the role of black carbon in the climate system: A scientific assessment,” J. Geophys. Res. Atmos. 118, 5380–5552 (2013).

Zheng, J.

A. F. Khalizov, H. Xue, L. Wang, J. Zheng, and R. Zhang, “Enhanced light absorption and scattering by carbon soot aerosol internally mixed with sulfuric acid,” J. Phys. Chem. A 113, 1066–1074 (2009).
[Crossref] [PubMed]

Zheng, L.

Y. Wu, T. Cheng, X. Gu, L. Zheng, H. Chen, and H. Xu, “The single scattering properties of soot aggregates with concentric core–shell spherical monomers,” J. Quant. Spectrosc. Radiat. Transfer 135, 9–19 (2014).
[Crossref]

Zuberi, B.

K. S. Johnson, B. Zuberi, L. T. Molina, M. J. Molina, M. J. Iedema, J. P. Cowin, D. J. Gaspar, C. Wang, and A. Laskin, “Processing of soot in an urban environment: case study from the Mexico City Metropolitan Area,” Atmos. Chem. Phys. 5, 3033–3043 (2005).
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Atmos. Chem. Phys. Discuss. (1)

P. R. Buseck, K. Adachi, A. Gelencsér, É. Tompa, and M. Po’sfai, “Are black carbon and soot the same?” Atmos. Chem. Phys. Discuss. 12, 24821–24846 (2012).

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Figures (12)

Fig. 1
Fig. 1 Transmission electron microscope images of (a) freshly emitted black carbon (BC) particles [40], (b) thinly coated light absorbing carbon aerosols [41], and (c) heavily coated light absorbing carbon aerosols [26].
Fig. 2
Fig. 2 Schematic diagram showing the transformation of light absorbing carbon aggregates with increasing mass fraction of condensed materials: (a) freshly emitted black carbon (BC) particles, (b) thinly coated light absorbing carbon aerosols, (c) heavily coated light absorbing carbon aerosols.
Fig. 3
Fig. 3 Absorption cross sections (Cabs) of internally mixed light absorbing carbon aerosols with various morphological factors: freshly emitted BC particles (Df = 2.0, S/C = 1.0), thinly coated light absorbing carbon aerosols (Df = 2.4, S/C = 1.5), and heavily coated light absorbing carbon aerosols (Df = 2.8, S/C = 2.0).
Fig. 4
Fig. 4 Single scattering albedo (SSA) and asymmetry parameter (ASY) of internally mixed light absorbing carbon aerosols with various morphological factors: freshly emitted black carbon particles (Df = 2.0, S/C = 1.0), thinly coated light absorbing carbon aerosols (Df = 2.4, S/C = 1.5), and heavily coated light absorbing carbon aerosols (Df = 2.8, S/C = 2.0).
Fig. 5
Fig. 5 Absorption cross sections of internally mixed light absorbing carbon aerosols with various shell/core ratio (S/C): (a) thinly coated light absorbing carbon aerosol (Df = 2.4, S/C = 1.1, 1.3, 1.5), (b) heavily coated light absorbing carbon aerosol (Df = 2.8, S/C = 1.5, 1.75, 2.0).
Fig. 6
Fig. 6 Single scattering albedo (SSA) and asymmetry parameter (ASY) of thinly coated light absorbing carbon aerosols with various shell/core ratio (S/C). Df = 2.4, S/C = 1.1, 1.3, 1.5.
Fig. 7
Fig. 7 Single scattering albedo (SSA) and asymmetry parameter (ASY) of heavily coated light absorbing carbon aerosols with various shell/core ratio (S/C). Df = 2.8, S/C = 1.5, 1.75, 2.0.
Fig. 8
Fig. 8 Absorption cross sections of internally mixed light absorbing carbon aerosols with various fractal dimensions (Df): (a) thinly coated light absorbing carbon aerosol (Df = 2.2, 2.4, 2.6, S/C = 1.5), (b) heavily coated light absorbing carbon aerosol (Df = 2.6, 2.8, 3.0, S/C = 1.75).
Fig. 9
Fig. 9 Single scattering albedo (SSA) and asymmetry parameter (ASY) of thinly coated light absorbing carbon aerosols with various fractal dimensions (Df = 2.2, 2.4, 2.6, S/C = 1.5)
Fig. 10
Fig. 10 Single scattering albedo (SSA) and asymmetry parameter (ASY) of heavily coated light absorbing carbon aerosols with various fractal dimensions (Df = 2.6, 2.8, 3.0, S/C = 1.75)
Fig. 11
Fig. 11 Ranges for optical properties of thinly coated light absorbing carbon aerosols with alterations due to assumption of the concentric spherical core-shell model (Df = 2.4, S/C = 1.1, 1.3, 1.5).
Fig. 12
Fig. 12 Ranges for optical properties of heavily coated light absorbing carbon aerosols with alteration due to assumption of the concentric spherical core-shell model (Df = 2.8, S/C = 1.5, 1.75, 2.0).

Tables (1)

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Table 1 Morphological Properties of Internally Mixed Light Absorbing Carbon Aerosols

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