Optical Properties and Radiative Forcing of Aged BC due to Hygroscopic Growth: Effects of the Aggregate Structure

Zeng, Chen; Liu, Chao; Li, Jiangnan; Zhu, Bin; Yin, Yan; Wang, Yuan

doi:10.1029/2018jd029809

Cited by 32 publications

(28 citation statements)

References 78 publications

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“…Exposure to humidity and coatings can collapse the BCFA into a structure having even a larger fractal dimension up to 2.6. (Zhang et al, 2008;Bambha et al, 2013). Hence, studying BC particles under the assumption of aggregate morphology provides a wider range of parameter space (particle size, primary particle size, and morphology).…”

Section: Morphology Of Bcfasmentioning

confidence: 99%

“…Various ambient and laboratory studies have emphasized the role of organic external coating in influencing BC absorption and scattering properties (Zhang et al, 2008;Ouf et al, 2016;Dong et al, 2018;Shiraiwa et al, 2010). However, previous modelling-based studies were not able to take into account information about the coating of the BCFAs.…”

Section: Introductionmentioning

confidence: 99%

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

et al. 2021

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

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Section: Morphology Of Bcfasmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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

et al. 2021

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“…diative forcing of BC aerosols with and without considering minor structures. We perform a simple radiative transfer simulation for a semiquantitative discussion, and the Santa Barbara DISORT Atmospheric Radiative Transfer Model is used to calculate BC forcing at a visible wavelength (Ricchiazzi et al, 1998;Zeng et al, 2019). Similar to the settings used by Zeng et al (2019), the midlatitude summer atmosphere profile is considered, and the surface albedo is set to 0.15.…”

Section: Effects Of Minor Structuresmentioning

confidence: 99%

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

et al. 2019

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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.

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“…The morphology of BC particles change markedly during atmospheric aging, with associated impacts on the particle size and optical properties (Zeng et al, 2019;Zhang et al, 2008;Teoh et al, 2019). In this study, the dynamic shape factor of BC particles and the material density of organic aerosols were derived by measuring the mass and/or mobility diameter of AACselected particles.…”

Section: Physical Properties Of Black Carbon and Organic Aerosolsmentioning

confidence: 99%

Physical and chemical properties of black carbon and organic matter from different sources using aerodynamic aerosol classification

Alfarra

Szpek

et al. 2021

Preprint

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Abstract. The physical and chemical properties of black carbon (BC) and organic aerosols are important for predicting their radiative forcing in the atmosphere. During the Soot Aerodynamic Size Selection for Optical properties (SASSO) project and a EUROCHAMP-2020 transnational access project, different types of light absorbing carbon were studied, including BC from catalytically stripped diesel exhaust, a flame burner, a colloidal graphite standard (Aquadag), and from controlled flaming wood combustion. Brown carbon (BrC) was also investigated in the form of organic aerosol emissions from wood burning (pyrolysis and smouldering) and from the nitration of secondary organic aerosol (SOA) proxies produced in a photochemical reaction chamber. Here we present insights into the physical and chemical properties of the aerosols, with optical properties being presented in subsequent publications. The dynamic shape factor (χ) of BC particles and material density (ρm) of organic aerosols were investigated by coupling a charging-free Aerodynamic Aerosol Classifier (AAC) with a Centrifugal Particle Mass Analyzer (CPMA) and Scanning Mobility Particle Sizer (SMPS). The morphology of BC particles was captured by transmission electron microscopy (TEM). For BC particles from the diesel engine and flame burner emissions, the primary spherule sizes were similar, around 20 nm. With increasing particle size, BC particles adopted more collapsed/compacted morphologies for the former source but tended to show more aggregated morphologies for the latter source. For particles emitted from the combustion of dry wood samples, the χ of BC particles and the ρm of organic aerosols were observed in the ranges 1.8–2.17 and 1.22–1.32 g/cm3, respectively. Similarly, for wet wood samples, the χ and ρm ranges were 1.2–1.85 and 1.44–1.60 g/cm3, respectively. Aerosol mass spectrometry measurements show no clear difference in mass spectra of the organic aerosols in individual burn phases (pyrolysis or smouldering phase) with the moisture content of the wood samples. This implies that the effect moisture has on the organic chemical profile of wood burning emissions is through changing the durations of the different phases of the burn cycle, not through the chemical modification of the individual phases. In this study, the incandescence signal of a Single Particle Soot Photometer (SP2) was calibrated with three different types of BC particles and compared with that from an Aquadag standard that is commonly used to calibrate SP2 incandescence to a BC mass. A correction factor is defined as the ratio of the incandescence signal from an alternative BC source to that from the Aquadag standard, and took values of 0.82 (or 0.79), 0.88 and 0.84–0.91 for the BC particles emitted from the diesel engine running under hot (or cold idle) conditions, the flame burner and wood combustion, respectively. These correction factors account for differences in instrument response to BC from different sources compared to the standardised Aquadag calibration and are more appropriate than the common value of 0.75 recommended by Laborde et al. (2012b) when deriving the mass concentration of BC emitted from diesel engines. Quantifying the correction factor for many types of BC particles found commonly in the atmosphere may enable better constraints to be placed on this factor depending on the BC source being sampled, and thus improve the accuracy of future SP2 measurements of BC mass concentrations.

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Optical Properties and Radiative Forcing of Aged BC due to Hygroscopic Growth: Effects of the Aggregate Structure

Cited by 32 publications

References 78 publications

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

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

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

Physical and chemical properties of black carbon and organic matter from different sources using aerodynamic aerosol classification

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