Black Carbon Optical Properties Research Articles

New insights into black carbon light absorption enhancement: A comprehensive analysis of two differential behaviors

High uncertainty in optical properties of black carbon (BC) involving heterogeneous chemistry has recently attracted increasing attention in the field of atmospheric climatology. To fill the gap in BC optical knowledge so as to estimate more accurate climate effects and serve the response to global warming, it is beneficial to conduct site-level studies on BC light absorption enhancement (Eabs) characteristics. Real-time surface gas and particulate pollutant observations during the summer and winter over Wuhan were utilized for the analysis of Eabs simulated by minimum R squared (MRS), considering two distinct atmospheric conditions (2015 and 2017). In general, differences in aerosol emissions led to Eabs differential behaviors. The summer average of Eabs (1.92 ± 0.55) in 2015 was higher than the winter average (1.27 ± 0.42), while the average (1.11 ± 0.20) in 2017 summer was lower than that (1.67 ± 0.69) in winter. Eabs and RBC (representing the mass ratio of non-refractory constituents to elemental carbon) constraints suggest that Eabs increased with the increase in RBC under the ambient condition enriched by secondary inorganic aerosol (SIA), with a maximum growth rate of 70.6% in 2015 summer. However, Eabs demonstrated a negative trend against RBC in 2017 winter due to the more complicated mixing state. The result arose from the opposite impact of hygroscopic SIA and absorbing OC/irregular distributed coatings on amplifying the light absorbency of BC. Furthermore, sensitivity analysis revealed a robust positive correlation (R > 0.9) between aerosol chemical compositions (including sulfate, nitrate, ammonium and secondary organic carbon), which could be significantly perturbed by only a small fraction of absorbing materials or restructuring BC through gaps filling. The above findings not only deepen the understanding of BC, but also provide useful information for the scientific decision-making in government to mitigate particulate pollution and obtain more precise BC radiative forcing.

Assessment of Black Carbon, optical properties and aerosol radiative forcing at Pranmati basin Himalayan critical zone observatory

The study aimed to understand the optical properties of Black Carbon (BC) and radiative forcing over a data deficient Himalayan region focusing on critical zone observatory employing ground-based measurements by Aethalometer for BC and satellite retrieval techniques for optical properties during mid-May-June 2022 and January–May 2023.BC mass concentration ranged from 0.18 to 4.43 μgm−3, exhibit a mean of 1.47 ± 0.83 μgm−3 with higher summer concentration (1.51 ± 0.94 μgm−3) than winter (1.39 ± 0.61 μgm−3). The average Absorption Ångström Exponent observed to be significantly higher than unity (1.77 ± 0.31) over the studied high-altitude Himalayan region, suggesting the dominance of biomass-burning aerosol. Higher aethalometer derived compensation parameter (K) in winter suggesting locally originated BC while, lower K value in summer suggesting aged BC transported from Indo-Gangetic Plains.Optical properties calculated from “Optical Properties of Aerosol and Cloud” (OPAC) model are used in the “Santa Barbara DISORT Atmospheric Radiative Transfer” (SBDART) model to calculate the aerosol Direct Radiative Force (DRF). The entire studied period is characterized by the predominance of absorbing aerosols, particularly BC, increasing Aerosol Optical Depth, Asymmetric Parameters and decreasing Single Scattering Albedo, leading to a considerable increase in atmospheric radiative forcing (+0.9 Wm−2, top of atmosphere) and Heating Rate (0.36 KDay−1). The mean radiative forcing within atmosphere during summer was higher (+14.29 Wm−2) relative to the winter (+12.00 Wm−2), emphasizing the impact of absorbing aerosols on regional warming and potential glacier melting in the Himalayas at a faster rate. Urgent policy consideration for the reduction of absorbing aerosols is highlighted, recognizing the critical roles of Black Carbon in the changing behaviour of Critical Zone observatory. The study's data serve as a valuable resource to understanding and addressing uncertainties in climate models, aiding effective policy implementation for Black Carbon reduction.

Roles of water-soluble aerosol coatings for the enhanced radiative absorption of black carbon over south asia and the northern indian ocean

Black Carbon (BC), formed by incomplete combustion, absorbs solar radiation and heats the atmosphere. We investigated the enhancement in optical absorption of BC due to coatings of water-soluble (WS) species in the polluted South Asian atmosphere. The BC Mass Absorption Cross-section (MAC; 678 nm) was estimated before and after removal of the WS components. Wintertime samples were collected from three South Asian receptor observatories intercepting large-footprint outflow: Bangladesh Climate Observatory Bhola (BCOB; integrating outflow of the Indo-Gangetic Plain), Maldives Climate Observatories at Hanimaadhoo (MCOH) and at Gan (MCOG), both reflecting outflow from the South Asian region. The ambient MAC observed at BCOB, MCOH and MCOG were 4.2 ± 1.4, 7.9 ± 1.9 and 7.1 ± 1.5 m2 g−1, respectively.The average enhancement of the BC MAC due to WS coatings (i.e., ws-EMAC) was identical at all three sites (1.6 ± 0.5) indicating that the anthropogenic aerosols had already evolved to a fully coated morphology at BCOB and/or that subsequent aging involved two compensating evolution processes of the coating. Inspecting the key coating component sulfate; the sulfate-to-BC ratio increased threefold when transitioning from BCOB to MCOH and by about 1.5 times from BCOB to MCOG. Conversely, both WS organic carbon (WSOC)/BC and water-insoluble OC (WIOC)/BC ratios declined with distance: WSOC/BC diminished by 84 % from BCOB to MCOH and by 80 % from BCOB to MCOG, while WIOC/BC dropped by about 63 % and 59 %, respectively. Such declines in WSOC and WIOC reflect a combination of photochemical oxidation and more efficient washout of OC compared to BC. The observed changes in the SO42−/BC and WSOC/BC ratios across South Asia highlight the significant impact of aerosol composition on the optical properties of Black Carbon (BC). These findings emphasize the need for detailed studies on aerosol composition to improve climate models and develop effective strategies for reducing the impact of anthropogenic aerosols on the climate.

Source-specified atmospheric age distribution of black carbon and its impact on optical properties over the Yangtze River Delta

Black carbon (BC) exerts a profound and intricate impact on both air quality and climate due to its high light absorption. However, the uncertainty in representing the absorption enhancement of BC in climate models leads to an increased range in the modeled aerosol climate effects. Changes in BC optical properties could result either from atmospheric aging processes or from variations in its sources. In this study, a source-age model for identifying emission sources and aging states presented by University of California at Davis/California Institute of Technology (UCD/CIT) was used to simulate the atmospheric age distribution of BC from different sources and to quantify its impact on the optical properties of BC-containing particles. The results indicate that regions with greater aged BC concentrations do not correspond to regions with higher BC emissions due to atmospheric transport. High concentrations of aged BC are found in northern Yangtze River Delta (YRD) regions during summer. The chemical compositions of particles from different sources and with different atmospheric ages differ significantly. BC and primary organic aerosols (POA) are dominating in Traffic-dominated source while other components dominate in Industry-dominated source. As the atmospheric age increases, the mass fraction of secondary inorganic aerosols rises. Compared to the original model, the simulated mass absorption cross section of BC particles in the source-age model decreases while the single scattering albedo increases. This compensates for ~11 % of the overestimation of the simulated BC direct radiative forcing. Our study highlights that incorporating atmospheric age and source information into models can greatly improve the estimation of optical properties of BC-containing particles and deepen our understanding of their climate effects.

Impacts of α-pinene ozonolysis products on the morphology and optical properties of black carbon

Black carbon (BC) is known to absorb solar radiation and thus have a warming impact on climate. The atmospheric aging of fresh BC has been suggested to enhance BC's light absorption, but the extent of variation observed varies largely in field and laboratory measurements. Biogenic VOCs with much higher abundance than anthropogenic emissions are reactive towards atmospheric oxidants, and act as major sources of secondary organic aerosol (SOA) in the atmosphere. In this study, we performed experiments of BC aging in the presence of condensable organic vapors generated from the ozonolysis of α-pinene. Significant changes in the particle size, mass, effective density, morphology as well as optical properties are observed upon coating of BC by α-pinene ozonolysis products. While the BC aging rate depends on the initial concentrations of precursors forming condensable materials and the particle size, the extent of transformation of BC at a given size is mainly controlled by the volume equivalent coating thickness. The highly fractal BC core is converted to a more compact morphology for a coating thickness of ∼25–30 nm depending on the initial particle size. The absorption and scattering of light by BC also increase by more than 1.29- and 5.30- fold during the coating process. The enhancement of optical properties can be attributed to both formation of coatings and restructuring of the BC core, with the latter accounting for a large fraction of optical enhancement. Our results indicate that the ozonolysis of α-pinene has profound effects on the morphology and optical properties of BC, with a magnitude comparable to sulfuric acid and ammonium nitrate, but much higher than other reported anthropogenic hydrocarbons. Although present in relatively low concentrations, α-pinene oxidation reactions can considerably enhance the impacts of BC on air quality and climate forcing.

Influence of Absorbing and Non-Absorbing Coating on Black Carbon Optical Properties at Different Coating Thickness

Influence of Absorbing and Non-Absorbing Coating on Black Carbon Optical Properties at Different Coating Thickness

Importance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations

Abstract. Black carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles, which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parameterization schemes for the optical properties of BC, using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. The modelling techniques were examined for bare BC particles in the first step and for BC particles with organic material in the second step. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. In general, the aggregate representation performed well for modelling the particle light absorption coefficient σabs, single-scattering albedo SSA, and mass absorption cross-section MACBC for laboratory-generated BC particles with volume mean mobility diameters dp,V larger than 100 nm. However, for modelling Ångström absorption exponent AAE, it was difficult to suggest a method due to size dependence, although the spherical assumption was in better agreement in some cases. The BC fractal aggregates are usually modelled using monodispersed particles, since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25 % uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the uncertainty in measured σabs to 10 % for particles with dp,V between 60–160 nm. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. When the BC particle is small and rather fresh, the change in the Df had relatively little effect on the optical properties. There was, however, a significant relationship between app and the particle light scattering, which increased by a factor of up to 6 with increasing total particle size. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 and 2, mim between 0.50 and 1, Df from 1.7 to 1.9, and app between 10 and 14 nm. Overall, this study provides experimental support for emphasizing the importance of an appropriate size representation (polydisperse size method) and an appropriate morphological representation for optical modelling and parameterization scheme development of BC.

Optical Properties of Black Carbon Aerosols with Different Coating Models

Research on the optical properties of black carbon (BC) aerosols is highly important for investigating global climate change. A general inhomogeneous particle superposition model is developed. Inhomogeneous particles with arbitrary shapes can be constructed by this model. BC aerosols with core-shell, spherical, ellipsoid, and irregular coating models are established to explore the impact of coating shape on their optical properties. The optical properties are studied employing the discrete dipole approximation method (DDA). The influences of the morphology of BC aerosols, the coating volume fractions, and the shape of coatings on the optical properties are analyzed. The irregular coating shape causes a higher forward scattering intensity and a lower extinction cross-section. The forward scattering intensity of the core-shell model is lower than other models. The effect of the coating shape on forward scattering intensity becomes smaller as coating volume and fractal dimension increase. Consequently, assuming irregular coating as spherical coating models considered in most studies leads to inaccuracy in the optical properties of BC aerosols. It is necessary to comprehensively consider the effects of aerosol morphology and coating volume for investigating the optical properties of black carbon aerosols.

Analysis of the Effect of Optical Properties of Black Carbon on Ozone in an Urban Environment at the Yangtze River Delta, China

Black carbon (BC) reduces the photolysis coefficient by absorbing solar radiation, thereby affecting the concentration of ozone (O3) near the ground. The influence of BC on O3 has thus received much attention. In this study, Mie scattering and the tropospheric Ultraviolet and Visible radiation model are used to analyze the effect of BC optical properties on radiation. Combined with data of O3 precursors in Nanjing in 2014, an EKMA curve is drawn, and the variations in O3 concentration are further investigated using a zero-dimensional box mechanism model (NCAR MM). When O3 precursors are unchanged, radiation and O3 show a highly similar tendency in response to changing BC optical properties (R=0.997). With the increase of modal radius, the attenuation of fresh BC to radiation and O3 first trends upward before decreasing. In the mixing process, the attenuation of BC to radiation and O3 presents an upward tendency with the increase of relative humidity but decreases rapidly before increasing slowly with increasing thickness of coating. In addition, mass concentration is another major factor. When the BC to PM2.5 ratio increases to 5% in Nanjing, the radiation decreases by approximately 0.13%–3.71% while O3 decreases by approximately 8.13%–13.11%. The radiative effect of BC not only reduces O3 concentration but also changes the EKMA curve. Compared with the NOx control area, radiation has a significant influence on the VOCs control area. When aerosol optical depth (AOD) increases by 17.15%, the NOx to VOCs ratio decreases by 8.27%, and part of the original NOx control area is transferred to the VOCs control area.

Atmospheric aerosol and black carbon optical properties and associated radiative forcing under haze conditions

The optical properties and radiative forcing of atmospheric aerosol (ARF) and black carbon (BC) aerosol (BCRF) in ultraviolet (UV), visible (VIS), near-infrared (NIR), and shortwave (SW) spectra were investigated under haze conditions based on the observations of the Aethalometer and sun-sky radiometer and simulations from libRadtran. The results show that the BC concentrations increased greatly from 2.73 μg/m3 under clear-air conditions to 7.95 μg/m3 under severe haze conditions, while BC aerosol optical depth (AOD) increased from 0.025 to 0.092. A high correlation (R2=0.62) was found between BC AOD and absorbing aerosol optical depth (AAOD) derived from the sun-sky radiometer. The BCRF in SW (BCRFSW) varied from -10.20 W/m2 under clear-air conditions to -25.40 W/m2 under severe hazy conditions. However, its fraction in ARF (ARFSW) decreased from 19% to 17% simultaneously, which is mainly related to the decrease of the ratio of BC AOD to AOD. The fraction of ARF in VIS in ARFSW decreased from 56.3% under clear-air conditions to 50.5% under severe haze conditions, while the fraction of BCRF in VIS in BCRFSW was much larger, and increased from 72.9% to 73.8%. The BCRF efficiency (BCRFE) was much larger than ARF efficiency (ARFE), and both of them decreased with the development of haze. The ARFE in SW decreased from -173.84 W/m2 under clear-air conditions to -112.75 W/m2 under severe haze conditions while BCRFESW varied from -482.50 W/m2 to -321.88 W/m2. The decrease of ARFE and BCRFE is related to the increase of aerosol loading and asymmetry factor (ASY). The ASY increased and the forward scattering was enhanced with the development of haze due to the hygroscopic growth of aerosol particles, which reduced the extinction efficiency of aerosols including BC on solar radiation and the cooling effect on the surface.

Simulated aging processes of black carbon and its impact during a severe winter haze event in the Beijing-Tianjin-Hebei region

Black carbon (BC) can mitigate or worsen air pollution by perturbing meteorological conditions. BC aging processes strongly influence the evolution of the particle size, concentration, and optical properties of BC, which determine its influence on meteorology. Here, we use the online coupled Weather Research and Forecasting-Chemistry (WRF-Chem) model to quantify the role of BC aging processes, including physical processes (PP) and absorption enhancement (AE), in causing BC-induced meteorological changes and their associated feedbacks to PM2.5 (particulate matter less than 2.5 μm in diameter) and O3 concentrations during a severe haze event in the Beijing-Tianjin-Hebei (BTH) region during 21–27 February 2014. Our results show that, compared to those from the simulation without PP, the simulated near-surface BC concentration and BC mass loading in the BTH region decreased by 6.6% and 12.1%, respectively, when PP were included. PP increased the proportion of large BC (particle diameter greater than 0.312 μm) below 1000 m from 28 to 33% to 59–64% in the BTH region. When both PP and AE were included in the simulation, the reduction in PBL height due to the BC-PBL interaction was 116.3 m (20.7%), compared to reductions of 75.7 m (13.5%) without AE and 66.6 m (11.9%) without PP and AE. However, during this haze event, anomalous northeasterly winds were produced by the direct radiative effect of BC, which further affected aerosol mixing and transport. Due to their combined impacts on multiple meteorological factors, the direct radiative effects of BC without PP and AE, without AE, and with PP and AE increased the surface concentrations of PM2.5 by 8.3 μg m−3 (by 6.1% relative to the mean value), 6.1 μg m−3 (4.5%) and 9.6 μg m−3 (7.0%), respectively, but decreased the surface O3 concentrations by 2.8 ppbv (7.4%), 4.0 ppbv (9.0%) and 5.0 ppbv (10.8%) on average in the BTH region during 21–27 February 2014.

The Angstrom exponents of black carbon aerosols with non-absorptive coating: A numerical investigation

Black carbon (BC) aerosols exert important effects on regional and global climate, whilst there still are significant uncertainties in their optical properties, particularly the spectral varying Angstrom exponents. This study numerically evaluates the influences of coating morphologies on optical properties of BC with non-absorbing coating, and evaluates the sensitivity of their Angstrom exponents, including extinction Angstrom exponent (EAE), absorption Angstrom exponent (AAE) and single scattering albedo Angstrom exponent (SSAAE), to particle microphysics with the multiple-sphere T-matrix method. Among all microphysical parameters, the shell/core ratio and size distribution play substantial roles in determining the EAE, AAE and SSAAE of coated BC, wherein the dependences of the Angstrom exponents on size distribution are higher. The EAE, AAE and SSAAE of coated BC by non-absorptive materials with different particle size distributions change in ranges of 0.3–1.5, 0.3–2.5 and –0.1–0.9, respectively. The core-shell Mie model can hardly produce accurate results of the Angstrom exponents of coated BC particles, especially the AAE and SSAAE. Our study reveals that BC coated by non-absorbing materials with large size distribution of coated BC may show negative SSAAE values for some coating microphysics, indicating the limitation of separating brown carbon from black carbon with a criterion of negative SSAAE.

Absorption closure in highly aged biomass burning smoke

Abstract. The optical properties of black carbon (BC) are a major source of uncertainty in regional and global climate studies. In the past, detailed investigation of BC absorption has been hampered by systematic biases in the measurement instrumentation. We present airborne measurements of aerosol absorption and black carbon microphysical properties in highly aged biomass burning plumes measured 4–8 d from their source over the southeast Atlantic Ocean during CLARIFY-2017, using a suite of novel photoacoustic spectrometers to measure aerosol absorption at 405, 514, and 655 nm and a single-particle soot photometer to measure the BC mass concentration, size, and mixing state. These measurements are of sufficient quality and detail to provide constraint on optical schemes used in climate models for the first time in biomass burning plumes far from their source – an aerosol environment that is one of the most important climatically. The average absorption Ångström exponents (AAE) were 1.38 over the wavelength range from 405 to 514 nm and 0.88 over the range from 514 to 655 nm, suggesting that brown carbon (BrC) contributed to 11±2 % of absorption at 405 nm. The effective organic aerosol (OA) mass absorption coefficient (MAC) was 0.31±0.09 m2 g−1 at 405 nm. The BC particles were universally thickly coated, and almost no externally mixed BC particles were detected. The average MAC of BC was 20±4, 15±3, and 12±2 m2g−1 at wavelengths of 405, 514, and 655 nm respectively, with equivalent absorption enhancements of around 1.85±0.45 at all three wavelengths, suggesting that the thick coatings acted as a lens that enhanced light absorption by the BC. We compared the measured MAC and AAE values with those calculated using several optical models and absorption parameterisations that took the measured BC mass and mixing state as inputs. Homogeneous grey-sphere Mie models were only able to replicate MAC for some low (real and imaginary) values of the complex BC refractive index (mBC) at the shortest wavelength, but they would have to use unrealistically low values of mBC to accurately replicate the AAE. A core–shell Mie model was able to generate good agreement for MAC in the green–red end of the visible spectrum for most values of mBC. However, there are no possible values of mBC that produce MAC values that agree with our observations at all three wavelengths, due to a wavelength-dependent underestimation of the MAC of the underlying BC core. Four semiempirical parameterisations from the literature were also tested, linking the BC mixing state to either the MAC or absorption enhancement. Two of these schemes produced results that agreed within a few percent with the measured MAC at all three wavelengths, and the AAE agreed well when discounting the effects of BrC. Our results uniquely demonstrate the validity of absorption parameterisations, as well as the failings of Mie calculations, in this highly aged environment. We recommend that future work should conduct similar analyses in environments where BC has different properties; future studies should also investigate the impact of implementing these types of schemes within climate models as well as the impact of developing equivalent schemes for light scattering by soot particles at visible wavelengths.

Recent Progress in Impacts of Mixing State on Optical Properties of Black Carbon Aerosol

Black carbon (BC) exerts profound impacts on air quality and climate because of its high-absorption cross section over a broad band of solar spectrum. Non-BC materials coated on BC could alter the mixing state of BC particles and can considerably enhance its mass absorption coefficient. Quantification of this absorption enhancement remains a challenge due to incomplete understanding of the complex physical and chemical properties related to mixing states. In this paper, we summarize the recent progress in measurement and modeling studies on the BC mixing state and their effects on optical properties. Laboratory and field-based observations have shown that the transformation of a mixing state from a highly fractal nature to a more compact shape exhibits a decrease in electric mobility diameter but an increase in fractal dimension and effective density. Meanwhile, the transition behavior is also obviously influenced by emission source which can determine the components of BC mixtures. Based on the empirically determined parameters, accurate numerical modeling shows great capability on calculating BC optical properties. However, considering the significant uncertainties related to BC microphysical properties, proper parameterization considering realistic BC aggregates and coating fraction can help to understand the progress from an externally to internally mixed state.

Size-resolved mixing state and optical properties of black carbon at an urban site in Beijing

The size-resolved (200–700 nm) mixing state and optical properties of black carbon (BC) in Beijing in the spring of 2019 were investigated using a tandem system consisting of an aerodynamic aerosol classifier, a nephelometer, and a single particle soot photometer. The results showed that the coating thickness distribution exhibited a clear bimodal pattern for BC-containing particles with a fixed aerodynamic diameter (Dae). Based on the coating thickness, BC-containing particles can be classified as having external and internal mixing states. The number fraction of internal BC-containing particles increases with increasing Dae and reaches 95% when Dae = 700 nm. Both the BC core diameter and coating thickness simultaneously increased with an increasing Dae of BC-containing particles. The dynamic shape factor (χ) of BC-containing particles decreased from 1.43 to 1.0 as Dae increased from 200 nm to 400 nm and varied around 1.0 when Dae = 500–700 nm. This demonstrated that thickly coated BC-containing particles were more likely to have regular shapes. An observation-constrained simulation on the basis of Mie theory showed that the coating plays an important role in light absorption. The amplification of BC absorption by the coating increased from 1.21 to 1.75 with increasing Dae due to the thicker coating of BC-containing particles with a larger Dae. The single-scattering albedo was dependent on size, increasing from 0.83 to 0.98 with increasing Dae. The size-dependent characteristics of BC-containing particles were similar under different pollution conditions, but BC-containing particles tended to be larger with a thicker coating and have a larger absorption enhancement under polluted conditions (PM2.5 > 75 μg/m3) than under clean conditions (PM2.5 < 35 μg/m3). This study highlights the strong dependence of the microphysical and optical properties of BC on size.

Atmospheric heating rate due to black carbon aerosols: Uncertainties and impact factors

This study investigates the impacts of black carbon (BC) properties (vertical concentration, shape, size, and mixing state) and atmospheric variables (cloud and aerosol loading, surface albedo, and solar zenith angle) on BC radiative effects. Observations from aircraft measurements, lidar, and the Aerosol Robotic Network (AERONET) are used to constrain BC and aerosol properties. The library for radiative transfer (Libradtran) model is used to calculate BC radiative forcing (RF). BC optical properties are obtained from numerical modeling with aggregate or spherical structures and different size distributions. By modifying the optical properties, different BC geometries and size distributions result in uncertainties in RF and heating rate less than 30%, while the uncertainty in heating rate due to different BC mixing states is as large as ~80%. The vertical distribution of BC concentrations explains less than 10% of the relative differences in RF and heating rate in the atmosphere, but can induce different heating rate vertical profiles, thus different planetary boundary layer (PBL) stabilities. Due to the significant influence of cloudy and aerosol conditions on incident solar radiation, atmospheric conditions play an important role in determining the BC heating rate. Meanwhile, the effects of surface albedo and solar zenith angle on the BC heating rate are most significantly near the surface. Taking the above factors into account, we introduce an empirical approximation of the BC heating rate to estimate its influence on the atmosphere. With the simple formula, the BC heating rate for a particular atmospheric layer can be approximated when the vertical condition is known, and this can be further applied to determine whether BC promotes or suppresses PBL development. Considering the importance of the BC vertical concentration in its heating rate, we suggest that light-absorbing aerosols and their vertical distributions must be better measured and modeled to improve the understanding of their radiative effects and interaction with PBL.

Concentrations, optical and radiative properties of carbonaceous aerosols over urban Lanzhou, a typical valley city: Results from in-situ observations and numerical model

The concentrations, optical and radiative effects of carbonaceous aerosols were essential to studies of the climatic, environmental and health effects. The previous studies less combined numerical simulation with in-situ observations, especially for the aerosol vertical profiles. In this study, we off-line measured vertical profiles of submicron black carbon (BC) aerosols and on-line obtained aerosol optical properties over urban Lanzhou during 26 December 2017 to 11 January 2018. The BC optical properties and radiative effects were evaluated using Optical Properties of Aerosols and Clouds (OPAC) and Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) models. The absorption and scattering coefficients and optical depth of BC aerosols ranged from 9 to 83 M m−1, 3–24 M m−1 and 0.02 to 0.2 respectively, which in average accounted for 50%, 3% and 11% of the optical properties of total aerosols during the study period. BC aerosol radiative forcing (ARF) within ATMOS (top-surface) varying from 16.6 to 108.8 W m−2 accounted for 17.3%–97.4% of total aerosols ARF with an average of 66.6%, and the percentages increased significantly as BC concentrations increased during the period. The mean atmospheric heating rate (AHR) induced by BC aerosols was 1.94 K day−1 ranging from 0.46 to 3.03 K day−1 during the study period. This study contributes to understanding the impacts of light-absorbing aerosols on climate and haze pollution in an urban valley.

Accounting for the effects of nonideal minor structures on the optical properties of black carbon aerosols

Abstract. Black carbon (BC) aerosol is the strongest sunlight-absorbing aerosol, and its optical properties are fundamental to radiative forcing estimations and retrievals of its size and concentration. BC particles exist as aggregate structures with small monomers and are widely represented by the idealized fractal aggregate model. In reality, BC particles possess complex and nonideal minor structures besides the overall aggregate structure, altering their optical properties in unforeseen ways. This study introduces the parameter “volume variation” to quantify and unify different minor structures and develops an empirical relationship to account for their effects on BC optical properties from those of ideal aggregates. Minor structures considered are as follows: the polydispersity of monomer size, the irregularity and coating of the individual monomer, and necking and overlapping among monomers. The discrete dipole approximation is used to calculate the optical properties of aggregates with these minor structures. Minor structures result in scattering cross-section enhancement slightly more than that of absorption cross section, and their effects on the angle-dependent phase matrix as well as asymmetry factor are negligible. As expected, the effects become weaker with the increase in wavelength. Our results suggest that a correction ratio of 1.05 is necessary to account for the mass or volume normalized absorption and scattering of nonideal aggregates in comparison to ideal ones, which also applies to aggregates with multiple minor structures. In other words, the effects of minor structures are mainly contributed by their influence on particle volume/mass that cannot be ignored, and a relative difference of approximately 5 % is noticed after removing the volume effects. Thus, accurate knowledge and evaluation of BC volume/mass are more important than those of the minor structures themselves. Most importantly, the simulations of optical properties of nonideal aggregates are greatly simplified by applying the empirical relationship because they can be directly obtained from those of the corresponding ideal aggregates, a volume/mass difference parameter, and the correction factor, i.e., 1.05, not the detailed minor structure information. We expect this convenient treatment to find wide applications for the accounting for the effects of nonideal minor structures on BC optical properties.

Improved Aerosol Processes and Effective Radiative Forcing in HadGEM3 and UKESM1

AbstractAerosol processes and, in particular, aerosol‐cloud interactions cut across the traditional physical‐Earth system boundary of coupled Earth system models and remain one of the key uncertainties in estimating anthropogenic radiative forcing of climate. Here we calculate the historical aerosol effective radiative forcing (ERF) in the HadGEM3‐GA7 climate model in order to assess the suitability of this model for inclusion in the UK Earth system model, UKESM1. The aerosol ERF, calculated for the year 2000 relative to 1850, is large and negative in the standard GA7 model leading to an unrealistic negative total anthropogenic forcing over the twentieth century. We show how underlying assumptions and missing processes in both the physical model and aerosol parameterizations lead to this large aerosol ERF. A number of model improvements are investigated to assess their impact on the aerosol ERF. These include an improved representation of cloud droplet spectral dispersion, updates to the aerosol activation scheme, and black carbon optical properties. One of the largest contributors to the aerosol forcing uncertainty is insufficient knowledge of the preindustrial aerosol climate. We evaluate the contribution of uncertainties in the natural marine emissions of dimethyl sulfide and organic aerosol to the ERF. The combination of model improvements derived from these studies weakens the aerosol ERF by up to 50% of the original value and leads to a total anthropogenic historical forcing more in line with assessed values.

Black carbon aggregates: A database for optical properties

Black carbon (BC) aerosol plays an important role in the atmosphere as an absorber of solar radiation and contributes significantly to global warming. The optical properties of BC are fundamental for both direct radiative effect studies and remote sensing of BC properties. However, due to the complex aggregation structures of BC particles, accurate simulations of their optical properties are limited and computationally expensive, while equivalent spherical models or approximate methods could easily introduce relative errors up to 30%. This study generates a comprehensive database to calculate aggregate optical properties efficiently and accurately. The database covers a wide range of BC properties including aggregation structure, refractive index, and particle size (both monomer size and number of monomers). An accurate numerical model, i.e. the multiple-sphere T-matrix method, is used to calculate the single-scattering properties of BC clusters in the form of fractal aggregates. By interpolation, the database can be used to give the scattering properties of aggregates with monomer number from 1 up to 3000, monomer size parameter from 0.05 to 0.5, real part of refractive index from 1.2 to 2.0, and imaginary part from 0.2 to 1.0. The relative errors caused by the interpolation are much less than 1% for the single scattering properties. The pre-calculated database and the implementation used to calculate the required aggregate optical properties are publicly available for users interested in remote sensing of BC aerosols and performing radiative effect calculations.