scholarly journals Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties

2015 ◽  
Vol 42 (4) ◽  
pp. 1243-1250 ◽  
Author(s):  
Swarup China ◽  
Barbara Scarnato ◽  
Robert C. Owen ◽  
Bo Zhang ◽  
Marian T. Ampadu ◽  
...  
Atmosphere ◽  
2020 ◽  
Vol 11 (1) ◽  
pp. 86
Author(s):  
Kangwei Li ◽  
Mingming Yan ◽  
Jiandong Shen ◽  
Xin Zhang ◽  
Chunmei Geng ◽  
...  

As atmospheric fresh soot particles age, they become coated with other chemical species. This transforms their physicochemical properties and affects their optical characteristics, which is of great importance to air quality, the environment and climate change. One of the predominantly occurring states of soot particles in the ambient environment is the core-shell mixing state. In this study, we used the core-shell model to calculate the optical absorption, scattering and extinction efficiency, absorption proportion and absorption exponent of coated soot particles. We then investigated the effects of different core sizes (D0), incident wavelengths (λ), coating materials and coating thicknesses on these optical characteristics. Absorption efficiency and absorption proportion of soot particles decreased as the coating became thicker, at core sizes of D0 = 20, 50 and 100 nm and λ = 405, 532 and 781 nm, regardless of the type of coating material. As the coating thickness increased, the absorption exponent (β) of inorganic-coated soot particles tended to rise and then fall, while the β value of organic-coated soot particles kept increasing. Our results advance our scientific understanding of the interaction of optical properties with chemical composition, mixing state, and aging processes of soot particles in the atmosphere.


2001 ◽  
Vol 32 ◽  
pp. 421-422
Author(s):  
K.-H. NAUMANN ◽  
H. SAATHOFF ◽  
M. SCHNAITER ◽  
U. SCHURATH

2018 ◽  
Vol 18 (16) ◽  
pp. 12141-12159 ◽  
Author(s):  
Sara D. Forestieri ◽  
Taylor M. Helgestad ◽  
Andrew T. Lambe ◽  
Lindsay Renbaum-Wolff ◽  
Daniel A. Lack ◽  
...  

Abstract. Optical properties of flame-generated black carbon (BC) containing soot particles were quantified at multiple wavelengths for particles produced using two different flames: a methane diffusion flame and an ethylene premixed flame. Measurements were made for (i) nascent soot particles, (ii) thermally denuded nascent particles, and (iii) particles that were coated and then thermally denuded, leading to the collapse of the initially lacy, fractal-like morphology. The measured mass absorption coefficients (MACs) depended on soot maturity and generation but were similar between flames for similar conditions. For mature soot, here corresponding to particles with volume-equivalent diameters >∼160 nm, the MAC and absorption Ångström exponent (AAE) values were independent of particle collapse while the single-scatter albedo increased. The MAC values for these larger particles were also size-independent. The mean MAC value at 532 nm for larger particles was 9.1±1.1 m2 g−1, about 17 % higher than that recommended by Bond and Bergstrom (2006), and the AAE was close to unity. Effective, theory-specific complex refractive index (RI) values are derived from the observations with two widely used methods: Lorenz–Mie theory and the Rayleigh–Debye–Gans (RDG) approximation. Mie theory systematically underpredicts the observed absorption cross sections at all wavelengths for larger particles (with x>0.9) independent of the complex RI used, while RDG provides good agreement. (The dimensionless size parameter x=πdp/λ, where dp is particle diameter and λ is wavelength.) Importantly, this implies that the use of Mie theory within air quality and climate models, as is common, likely leads to underpredictions in the absorption by BC, with the extent of underprediction depending on the assumed BC size distribution and complex RI used. We suggest that it is more appropriate to assume a constant, size-independent (but wavelength-specific) MAC to represent absorption by uncoated BC particles within models.


2012 ◽  
Vol 12 (10) ◽  
pp. 26401-26434 ◽  
Author(s):  
B. Scarnato ◽  
S. Vahidinia ◽  
D. T. Richard ◽  
T. W. Kirchstetter

Abstract. According to recent studies, internal mixing of black carbon (BC) with other aerosol materials in the atmosphere alters its aggregate shape, absorption of solar radiation, and radiative forcing. These mixing state effects are not yet fully understood. In this study, we characterize the morphology and mixing state of bare BC and BC internally mixed with sodium chloride (NaCl) using electron microscopy and examine the sensitivity of optical properties to BC mixing state and aggregate morphology using a discrete dipole approximation model (DDSCAT). DDSCAT predicts a higher mass absorption coefficient, lower single scattering albedo (SSA), and higher absorption Angstrom exponent (AAE) for bare BC aggregates that are lacy rather than compact. Predicted values of SSA at 550 nm range between 0.18 and 0.27 for lacy and compact aggregates, respectively, in agreement with reported experimental values of 0.25 ± 0.05. The variation in absorption with wavelength does not adhere precisely to a power law relationship over the 200 to 1000 nm range. Consequently, AAE values depend on the wavelength region over which they are computed. In the 300 to 550 nm range, AAE values ranged in this study from 0.70 for compact to 0.95 for lacy aggregates. The SSA of BC internally mixed with NaCl (100–300 nm in radius) is higher than for bare BC and increases with the embedding in the NaCl. Internally mixed BC SSA values decrease in the 200–400 nm wavelength range, a feature also common to the optical properties of dust and organics. Linear polarization features are also predicted in DDSCAT and are dependent on particle morphology. The bare BC (with a radius of 80 nm) presents in the linear polarization a bell shape feature, which is a characteristic of the Rayleigh regime (for particles smaller than the wavelength of incident radiation). When BC is internally mixed with NaCl (100–300 nm in radius), strong depolarization features for near-VIS incident radiation are evident, such as a decrease in the intensity and multiple modes at different angles corresponding to different mixing states. DDSCAT, being flexible on the geometry and refractive index of the particle, can be used to study the effect of mixing state and complex morphology on optical properties of realistic BC aggregates. This study shows that DDSCAT predicts morphology and mixing state dependent optical properties that have been reported previously and are relevant to radiative transfer and climate modeling and interpretation of remote sensing measurements.


Atmosphere ◽  
2019 ◽  
Vol 10 (4) ◽  
pp. 168 ◽  
Author(s):  
Robin Stevens ◽  
Ashu Dastoor

Aerosol mixing state significantly affects concentrations of cloud condensation nuclei (CCN), wet removal rates, thermodynamic properties, heterogeneous chemistry, and aerosol optical properties, with implications for human health and climate. Over the last two decades, significant research effort has gone into finding computationally-efficient methods for representing the most important aspects of aerosol mixing state in air pollution, weather prediction, and climate models. In this review, we summarize the interactions between mixing-state and aerosol hygroscopicity, optical properties, equilibrium thermodynamics and heterogeneous chemistry. We focus on the effects of simplified assumptions of aerosol mixing state on CCN concentrations, wet deposition, and aerosol absorption. We also summarize previous approaches for representing aerosol mixing state in atmospheric models, and we make recommendations regarding the representation of aerosol mixing state in future modelling studies.


2019 ◽  
Vol 19 (15) ◽  
pp. 10433-10446 ◽  
Author(s):  
Hua Yu ◽  
Weijun Li ◽  
Yangmei Zhang ◽  
Peter Tunved ◽  
Manuel Dall'Osto ◽  
...  

Abstract. Interaction of anthropogenic particles with radiation and clouds plays an important role in Arctic climate change. The mixing state of aerosols is a key parameter to influence aerosol radiation and aerosol–cloud interactions. However, little is known of this parameter in the Arctic, preventing an accurate representation of this information in global models. Here we used transmission electron microscopy with energy-dispersive X-ray spectrometry, scanning electron microscopy, nanoscale secondary ion mass spectrometry, and atomic forces microscopy to determine the size and mixing state of individual sulfate and carbonaceous particles at 100 nm to 2 µm collected in the Svalbard Archipelago in summer. We found that 74 % by number of non-sea-salt sulfate particles were coated with organic matter (OM); 20 % of sulfate particles also had soot inclusions which only appeared in the OM coating. The OM coating is estimated to contribute 63 % of the particle volume on average. To understand how OM coating influences optical properties of sulfate particles, a Mie core–shell model was applied to calculate optical properties of individual sulfate particles. Our result shows that the absorption cross section of individual OM-coated particles significantly increased when assuming the OM coating as light-absorbing brown carbon. Microscopic observations here suggest that OM modulates the mixing structure of fine Arctic sulfate particles, which may determine their hygroscopicity and optical properties.


2019 ◽  
Vol 12 (1) ◽  
pp. 107-118 ◽  
Author(s):  
Hiroshi Ishimoto ◽  
Rei Kudo ◽  
Kouji Adachi

Abstract. To retrieve the physical properties of aerosols from multi-channel ground-based and satellite measurements, we developed a shape model of coated soot particles and created a dataset of their optical properties. Bare soot particles were assumed to have an aggregate shape, and two types of aggregates with different size–shape dependences were modeled using a polyhedral Voronoi structure. To simulate the detailed shape properties of mixtures of soot aggregates and adhered water-soluble substances, we propose a simple model of surface tension derived from the artificial surface potential. The light-scattering properties of the modeled particles with different volume fractions of water-soluble material were calculated using the finite-difference time-domain method and discrete-dipole approximation. The results of the single-scattering albedo and asymmetry factors were compared to those of conventional internally mixed spheres (i.e., effective medium spheres based on the Maxwell-Garnett approximation and simple core-shell spheres). In addition, the lidar backscattering properties (i.e., lidar ratios and linear depolarization ratios) of the modeled soot particles were investigated. For internally mixed soot particles, the lidar backscattering properties were sensitive to the shape of the soot particles and the volume mixing ratio of the assumed water-soluble components. However, the average optical properties of biomass smoke, which have been reported from in situ field and laboratory measurements, were difficult to explain based on the individually modeled particle. Nonetheless, our shape model and its calculated optical properties are expected to be useful as an alternative model for biomass smoke particles in advanced remote sensing via multi-channel radiometer and lidar measurements.


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