scholarly journals Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition

2020 ◽  
Vol 117 (10) ◽  
pp. 5196-5203 ◽  
Author(s):  
Laura Fierce ◽  
Timothy B. Onasch ◽  
Christopher D. Cappa ◽  
Claudio Mazzoleni ◽  
Swarup China ◽  
...  

Black carbon (BC) absorbs solar radiation, leading to a strong but uncertain warming effect on climate. A key challenge in modeling and quantifying BC’s radiative effect on climate is predicting enhancements in light absorption that result from internal mixing between BC and other aerosol components. Modeling and laboratory studies show that BC, when mixed with other aerosol components, absorbs more strongly than pure, uncoated BC; however, some ambient observations suggest more variable and weaker absorption enhancement. We show that the lower-than-expected enhancements in ambient measurements result from a combination of two factors. First, the often used spherical, concentric core-shell approximation generally overestimates the absorption by BC. Second, and more importantly, inadequate consideration of heterogeneity in particle-to-particle composition engenders substantial overestimation in absorption by the total particle population, with greater heterogeneity associated with larger model–measurement differences. We show that accounting for these two effects—variability in per-particle composition and deviations from the core-shell approximation—reconciles absorption enhancement predictions with laboratory and field observations and resolves the apparent discrepancy. Furthermore, our consistent model framework provides a path forward for improving predictions of BC’s radiative effect on climate.

2015 ◽  
Vol 15 (14) ◽  
pp. 19835-19872 ◽  
Author(s):  
C. He ◽  
K.-N. Liou ◽  
Y. Takano ◽  
R. Zhang ◽  
M. L. Zamora ◽  
...  

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.


2019 ◽  
Author(s):  
Hang Liu ◽  
Xiaole Pan ◽  
Dantong Liu ◽  
Xiaoyong Liu ◽  
Xueshun Chen ◽  
...  

Abstract. Black carbon aerosols play an important role in climate change by absorbing solar radiation and degrading visibility. In this study, the mixing state of refractory black carbon (rBC) at an urban site in Beijing was studied with a single particle soot photometer (SP2), as well as a tandem observation system with a centrifugal particle mass analyzer (CPMA) and a differential mobility analyzer (DMA), in early summer of 2018. The results demonstrated that the mass-equivalent size distribution of rBC exhibited an approximately lognormal distribution with a mass median diameter (MMD) of 171.2 nm. When the site experienced prevailing southerly winds, the MMD of rBC increased notably by 19 %. During the observational period, the ratio of the diameter of rBC-containing particles (Dp) to the rBC core (Dc) was 1.20 on average for Dc = 180 nm, indicating that the majority of rBC particles were thinly coated. The Dp / Dc value exhibited a clear diurnal pattern, with a maximum at 1400 LST and an enhancing rate of 0.013/h; higher Ox conditions increased the coating enhancing rate. Bare rBC particles were primarily in a fractal structure with a mass fractal dimension (Dfm) of 2.35, with limited variation during both clean and pollution periods, indicating significant impacts from on-road vehicle emissions. The morphology of rBC-containing particles vairied with aging processes. The mixing state of rBC particles could be indicated by the mass ratio of non-refractory matter to rBC (MR). In the present study, rBC-containing particles were primarily found in an external fractal structure when MR  6, at which the measured scattering cross section of rBC-containing particles was consistent with that based on the Mie-scattering simulation. We found only 9 % of the rBC-containing particles were in core-shell structures on clean days with a particle mass of 10 fg, and the number fraction of core-shell structures increased considerably to 32 % on pollution days. Considering the morphology change, the absorption enhancement (Eabs) was 11.7 % higher based on core-shell structures. This study highlights the combined effects of morphology and coating thickness on the Eabs of rBC-containing particles, which will be helpful for determining the climatic effects of BC.


2010 ◽  
Vol 10 (9) ◽  
pp. 4207-4220 ◽  
Author(s):  
D. A. Lack ◽  
C. D. Cappa

Abstract. The presence of clear coatings on atmospheric black carbon (BC) particles is known to enhance the magnitude of light absorption by the BC cores. Based on calculations using core/shell Mie theory, we demonstrate that the enhancement of light absorption (EAbs) by atmospheric black carbon (BC) when it is coated in mildly absorbing material (CBrown) is reduced relative to the enhancement induced by non-absorbing coatings (CClear). This reduction, sensitive to both the CBrown coating thickness and imaginary refractive index (RI), can be up to 50% for 400 nm radiation and 25% averaged across the visible radiation spectrum for reasonable core/shell diameters. The enhanced direct radiative forcing possible due to the enhancement effect of CClear is therefore reduced if the coating is absorbing. Additionally, the need to explicitly treat BC as an internal, as opposed to external, mixture with CBrown is shown to be important to the calculated single scatter albedo only when models treat BC as large spherical cores (>50 nm). For smaller BC cores (or fractal agglomerates) consideration of the BC and CBrown as an external mixture leads to relatively small errors in the particle single scatter albedo of <0.03. It has often been assumed that observation of an absorption Angström exponent (AAE)>1 indicates absorption by a non-BC aerosol. Here, it is shown that BC cores coated in CClear can reasonably have an AAE of up to 1.6, a result that complicates the attribution of observed light absorption to CBrown within ambient particles. However, an AAE<1.6 does not exclude the possibility of CBrown; rather CBrown cannot be confidently assigned unless AAE>1.6. Comparison of these model results to various ambient AAE measurements demonstrates that large-scale attribution of CBrown is a challenging task using current in-situ measurement methods. We suggest that coincident measurements of particle core and shell sizes along with the AAE may be necessary to distinguish absorbing and non-absorbing OC.


2020 ◽  
Vol 20 (9) ◽  
pp. 5771-5785 ◽  
Author(s):  
Hang Liu ◽  
Xiaole Pan ◽  
Dantong Liu ◽  
Xiaoyong Liu ◽  
Xueshun Chen ◽  
...  

Abstract. Black carbon aerosols play an important role in climate change because they directly absorb solar radiation. In this study, the mixing state of refractory black carbon (rBC) at an urban site in Beijing in the early summer of 2018 was studied with a single-particle soot photometer (SP2) as well as a tandem observation system with a centrifugal particle mass analyzer (CPMA) and a differential mobility analyzer (DMA). The results demonstrated that the mass-equivalent size distribution of rBC exhibited an approximately lognormal distribution with a mass median diameter (MMD) of 171 nm. When the site experienced prevailing southerly winds, the MMD of rBC increased notably, by 19 %. During the observational period, the ratio of the diameter of rBC-containing particles (Dp) to the rBC core (Dc) was 1.20 on average for Dc=180 nm, indicating that the majority of rBC particles were thinly coated. The Dp∕Dc value exhibited a clear diurnal pattern, with a maximum at 14:00 LST and a Dp growth rate of 2.3 nm h−1; higher Ox conditions increased the coating growth rate. The microphysical properties of rBC were also studied. Bare rBC particles were mostly found in fractal structures with a mass fractal dimensions (Dfm) of 2.35, with limited variation during both clean and polluted periods. The morphology of rBC changed with coating thickness increasing. When the mass ratio of nonrefractory matter to rBC (MR) was <1.5, rBC-containing particles were primarily found in external fractal structures, and they changed to a core–shell structure when MR>6, at which point the measured scattering cross section of rBC-containing particles was consistent with that based on the Mie-scattering simulation. We found that only 28 % of the rBC-containing particles were in core–shell structures with a particle mass of 10 fg in the clean period but that proportion increased considerably, to 45 %, in the polluted period. Due to the morphology change, the absorption enhancement (Eabs) was 12 % lower than that predicted for core–shell structures.


2010 ◽  
Vol 10 (1) ◽  
pp. 785-819 ◽  
Author(s):  
D. A. Lack ◽  
C. D. Cappa

Abstract. The presence of clear coatings on atmospheric black carbon (BC) particles is known to enhance the magnitude of light absorption by the BC cores. Based on calculations using core/shell Mie theory, we demonstrate the enhancement of light absorption (EAbs) by atmospheric black carbon (BC) when coated in mildly absorbing material (CBrown) is reduced, relative to the enhancement by non-absorbing coatings (CClear). This reduction, sensitive to CBrown shell thickness and imaginary refractive index (RI), can be up to 50% for 400 nm radiation and 25% averaged across the visible radiation spectrum for reasonable core/shell diameters. The enhanced direct radiative forcing possible due to the enhancement effect of CClear is therefore reduced if the coating is absorbing. Additionally, the need to explicitly treat BC as an internal, as opposed to external, mixture with CBrown is shown to be important to the calculated single scatter albedo only whensub models treat BC as large spherical cores (>50 nm). For smaller BC cores (or fractal agglomerates) consideration of the BC and CBrown as an external mixture leads to relatively small errors in the particle single scatter albedo of <0.03. It is often assumed that observation of an absorption Angstrom exponent (AAE) >1 indicates non-BC absorption. Here, it is shown that BC cores coated in CClearcan reasonably have an AAE of up to 1.6, a result that complicates the attribution of observed light absorption to CBrown within ambient particles. However, an AAE<1.6 does not exclude the possibility of CBrown, rather CBrown cannot be confidently assigned unless AAE>1.6. Comparison of these results to some ambient AAE data shows that large-scale attribution of CBrown is a challenging task using current in-situ measurement methods. We suggest that coincident measurements of particle core and shell sizes along with the AAE may be necessary to distinguish absorbing and non-absorbing OC.


2018 ◽  
Vol 18 (15) ◽  
pp. 11345-11361 ◽  
Author(s):  
John K. Kodros ◽  
Sarah J. Hanna ◽  
Allan K. Bertram ◽  
W. Richard Leaitch ◽  
Hannes Schulz ◽  
...  

Abstract. Transport of anthropogenic aerosol into the Arctic in the spring months has the potential to affect regional climate; however, modeling estimates of the aerosol direct radiative effect (DRE) are sensitive to uncertainties in the mixing state of black carbon (BC). A common approach in previous modeling studies is to assume an entirely external mixture (all primarily scattering species are in separate particles from BC) or internal mixture (all primarily scattering species are mixed in the same particles as BC). To provide constraints on the size-resolved mixing state of BC, we use airborne single-particle soot photometer (SP2) and ultrahigh-sensitivity aerosol spectrometer (UHSAS) measurements from the Alfred Wegener Institute (AWI) Polar 6 flights from the NETCARE/PAMARCMIP2015 campaign to estimate coating thickness as a function of refractory BC (rBC) core diameter and the fraction of particles containing rBC in the springtime Canadian high Arctic. For rBC core diameters in the range of 140 to 220 nm, we find average coating thicknesses of approximately 45 to 40 nm, respectively, resulting in ratios of total particle diameter to rBC core diameters ranging from 1.6 to 1.4. For total particle diameters ranging from 175 to 730 nm, rBC-containing particle number fractions range from 16 % to 3 %, respectively. We combine the observed mixing-state constraints with simulated size-resolved aerosol mass and number distributions from GEOS-Chem–TOMAS to estimate the DRE with observed bounds on mixing state as opposed to assuming an entirely external or internal mixture. We find that the pan-Arctic average springtime DRE ranges from −1.65 to −1.34 W m−2 when assuming entirely externally or internally mixed BC. This range in DRE is reduced by over a factor of 2 (−1.59 to −1.45 W m−2) when using the observed mixing-state constraints. The difference in DRE between the two observed mixing-state constraints is due to an underestimation of BC mass fraction in the springtime Arctic in GEOS-Chem–TOMAS compared to Polar 6 observations. Measurements of mixing state provide important constraints for model estimates of DRE.


2018 ◽  
Author(s):  
John K. Kodros ◽  
Sarah Hanna ◽  
Allan Bertram ◽  
W. Richard Leaitch ◽  
Hannes Schulz ◽  
...  

Abstract. Transport of anthropogenic aerosol into the Arctic in the spring months has the potential to affect regional climate; however, modeling estimates of the aerosol direct radiative effect (DRE) are sensitive to uncertainties in the mixing state of black carbon (BC). A common approach in previous modeling studies is to assume an entirely external mixture (all primarily scattering species are in separate particles from BC) or internal mixture (all primarily scattering species are mixed in the same particles as BC). To provide constraints on the size-resolved mixing state of BC, we use airborne Single Particle Soot Photometer (SP2) and Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) measurements from the Alfred Wegener Institute (AWI) POLAR6 flights from the NETCARE/PAMARCMIP2015 campaign to estimate coating thickness as a function of refractory BC (rBC) core diameter as well as the fraction of particles containing rBC in the springtime Canadian high Arctic. For rBC core diameters in the range of 140 to 220 nm, we find average coating thicknesses of approximately 45 to 40 nm, respectively, resulting in ratios of total particle diameter to rBC core diameters ranging from 1.6 to 1.4. For total particle diameters ranging from 175 to 730 nm, rBC-containing particle number fractions range from 16 to 3 %, respectively. We combine the observed mixing-state constraints with simulated size-resolved aerosol mass and number distributions from GEOS-Chem-TOMAS to estimate the DRE with observed bounds on mixing state as opposed to assuming an entirely external or internal mixture. We find that the pan-Arctic average springtime DRE ranges from −1.65 W m−2 to −1.34 W m−2 when assuming entirely externally or internally mixed BC. Using the observed mixing-state constraints, we find the DRE is 0.05 W m−2 and 0.19 W m−2 less negative than the external mixing-state assumption when constraining by coating thickness of the mixed particles and by BC-containing particle number fraction, respectively. The difference between these methods is due to an underestimation of BC mass fraction in the springtime Arctic in GEOS-Chem-TOMAS compared to POLAR6 observations. Measurements of mixing state provide important constraints for model estimates of DRE.


2018 ◽  
Vol 18 (23) ◽  
pp. 16897-16914 ◽  
Author(s):  
Jie Luo ◽  
Yongming Zhang ◽  
Feng Wang ◽  
Qixing Zhang

Abstract. Using the numerically exact multiple sphere T-matrix (MSTM) method, we explored the effects of brown coatings on absorption enhancement (Eabs) of black carbon (BC) at different wavelengths (λ). In addition, the ratio of the absorption of BC coated by brown carbon (BrC) to an external mixture of BrC and BC (Eabs_internal) is also investigated. In this work, thinly coated BC is defined as that with a BC volume fraction over 20 %, and other BC is considered to be thickly coated. Eabs increases with the absorption of coatings, while an opposite trend is observed for Eabs_internal. A much wider range of Eabs is observed for BC with brown coatings compared to that with non-absorbing coatings. As the mass ratio of BrC to BC (MR) is over 13.9, Eabs can exceed 5.4 for BC with brown coatings at λ=0.35 µm under a typical size distribution. Specifically, as MR increases to approximately 13.9, Eabs values of larger than 3.96 can be observed at 0.532 µm, which is a little higher than the commonly measured Eabs of 1.05–3.5 at this wavelength. Previous studies have focused on the lensing effects of coatings but neglected the blocking effects of absorbing coatings. Eabs_internal can be below 1 at an ultraviolet spectral region for BC with brown coatings, which indicates that the absorption of internally mixed BC is less than that of an external mixture of BrC and BC due to the blocking effects of outer coatings, and we named the blocking effect of absorbing coatings the “sunglasses effect”. In addition, the applicability of a core–shell sphere model is also evaluated for BC with brown coatings. The absorption cross section (Cabs) of thickly coated BC is underestimated by the core–shell sphere model for all wavelengths while the underestimation becomes negligible as the imaginary part of the refractive index of brown carbon (kBrC) becomes very large. The lensing effect and the sunglasses effect are clearly defined. Moreover, the effects of composition ratios and the size distribution are explored at different wavelengths. Our findings can improve the understanding of the absorption enhancement of BC with brown coatings.


2019 ◽  
Vol 19 (1) ◽  
pp. 181-204 ◽  
Author(s):  
Gabriele Curci ◽  
Ummugulsum Alyuz ◽  
Rocio Barò ◽  
Roberto Bianconi ◽  
Johannes Bieser ◽  
...  

Abstract. An accurate simulation of the absorption properties is key for assessing the radiative effects of aerosol on meteorology and climate. The representation of how chemical species are mixed inside the particles (the mixing state) is one of the major uncertainty factors in the assessment of these effects. Here we compare aerosol optical properties simulations over Europe and North America, coordinated in the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII), to 1 year of AERONET sunphotometer retrievals, in an attempt to identify a mixing state representation that better reproduces the observed single scattering albedo and its spectral variation. We use a single post-processing tool (FlexAOD) to derive aerosol optical properties from simulated aerosol speciation profiles, and focus on the absorption enhancement of black carbon when it is internally mixed with more scattering material, discarding from the analysis scenes dominated by dust. We found that the single scattering albedo at 440 nm (ω0,440) is on average overestimated (underestimated) by 3–5 % when external (core-shell internal) mixing of particles is assumed, a bias comparable in magnitude with the typical variability of the quantity. The (unphysical) homogeneous internal mixing assumption underestimates ω0,440 by ∼14 %. The combination of external and core-shell configurations (partial internal mixing), parameterized using a simplified function of air mass aging, reduces the ω0,440 bias to -1/-3 %. The black carbon absorption enhancement (Eabs) in core-shell with respect to the externally mixed state is in the range 1.8–2.5, which is above the currently most accepted upper limit of ∼1.5. The partial internal mixing reduces Eabs to values more consistent with this limit. However, the spectral dependence of the absorption is not well reproduced, and the absorption Ångström exponent AAE675440 is overestimated by 70–120 %. Further testing against more comprehensive campaign data, including a full characterization of the aerosol profile in terms of chemical speciation, mixing state, and related optical properties, would help in putting a better constraint on these calculations.


2018 ◽  
Author(s):  
Gabriele Curci ◽  
Ummugulsum Alyuz ◽  
Rocio Barò ◽  
Roberto Bianconi ◽  
Johannes Bieser ◽  
...  

Abstract. An accurate simulation of the absorption properties is key for assessing the radiative effects of aerosol on meteorology and climate. The representation of how chemical species are mixed inside the particles (the mixing state) is one of the major uncertainty factors in the assessment of these effects. Here we compare aerosol optical properties simulations over Europe and North America, coordinated in the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII), to one year of AERONET sunphotometer retrievals, in an attempt to identify a mixing state representation that better reproduces the observed single scattering albedo and its spectral variation. We use a single post-processing tool (FlexAOD) to derive aerosol optical properties from simulated aerosol speciation profiles, and focus on the absorption enhancement of black carbon when it is internally mixed with more scattering material, discarding from the analysis scenes dominated by dust. We found that the single scattering albedo at 440 nm (ω0,440) is on average overestimated (underestimated) by 3–5 % when external (core-shell internal) mixing of particles is assumed, a bias comparable in magnitude with the typical variability of the quantity. The (unphysical) homogeneous internal mixing assumption underestimates ω0,440 by ~ 14 %. The combination of external and core-shell configurations (partial internal mixing), parameterized using a simplified function of air mass aging, reduces the ω0,440 bias to −1/−3 %. The black carbon absorption enhancement (Eabs) in core-shell with respect to the externally mixed state is in the range 1.8–2.5, which is above the currently most accepted upper limit of ~ 1.5. The partial internal mixing reduces Eabs to values more consistent with this limit. However, the spectral dependence of the absorption is not well reproduced, and the absorption Angostrom exponent AAE440675 is overestimated by 70–120 %. Further testing against more comprehensive campaign data, including a full characterization of the aerosol profile in terms of chemical speciation, mixing state, and related optical properties, would help in putting a better constraint on these calculations.


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