Orientation-averaged light-extinction characteristics of compound particles including aggregate effects

Orientation-averaged light-extinction characteristics of compound sulfate-carbon-soot particles have been analyzed with a discrete-dipole algorithm (DDSCAT code) for r1/r2 (ratio of primary-particle radius to secondary-particle radius) in the range 7 to 1 and for wavelengths from 0.4 to 0.8 microm. It was found that compound particles above a particle radius of approximately 0.2 microm exhibit light-extinction characteristics that closely match those of a pure sulfate particle. The shielding of the carbon particle by the primary particle apparently reduces the absorption effect of the soot particle over the range of all possible orientations. In light of the fact that soot particles tend to be small in comparison with host sulfate particles, the light-extinction characteristics of compound particles are dictated by the optical properties of the host particles. This result has been applied for aerosol aggregates with log-normal size distributions. For r1/r2 > or = 2 the aggregate extinction coefficient of a group of compound particles remains within 12% of that of a group consisting only of sulfate particles. This allows for effective calculation of the overall aerosol light extinction on the basis of the optical and geometrical properties of the constituent particles without having to include a compound-geometry effect.     

Electrostatics analysis of radiative absorption by sphere clusters in the Rayleigh limit: application to soot particles

An analysis of radiative absorption and scattering by clusters of spheres in the Rayleigh limit is developed with an electrostatics analysis. This approach assumes that the largest dimension of the cluster is significantly smaller than the wavelength of the radiation. The electric field that is incident upon and scattered by the cluster can then be represented by the gradient of a potential that in turn satisfies Laplace's equation. An analytical solution for the potential that exactly satisfies the boundary conditions at the surfaces of the spheres is obtained with a coupled spherical harmonics method. The components of the polarizability tensor and the absorption, scattering, and depolarization factors are obtained from the solution. Calculations are performed on fractallike clusters of spheres, with refractive-index values that are characteristic of carbonaceous soot in the visible and the IR wavelengths. Results indicate that the absorption cross sections of fractal soot clusters can be significantly larger in the mid-IR wavelengths than what is predicted for Rayleigh-limit spheres that have the same total volume. The absorption cross section (relative to a sphere of the same volume) is dependent on the number of spheres in the aggregate for aggregates with up to approximately 100 primary spheres, and for larger aggregates the relative absorption becomes constant. The predicted spectral variation of soot absorption in the visible and the mid-IR wavelengths is shown to agree well with experimental measurements.     

Effect of particle size ratio and contribution of particle size fractions on micromechanics of uniaxially compressed binary sphere mixtures

This paper is an extension of the recent work of Wi?cek (Granul Matter 18:42, 2016), wherein geometrical parameters of binary granular mixtures with various particle size ratio and contribution of the particle size fractions were investigated. In this study, a micromechanics of binary mixtures with various ratio of the diameter of small and large spheres and contribution of small particles was analyzed using discrete element simulations of confined uniaxial compression. The study addressed contact normal orientation distributions, global and partial contact force distributions and pressure distribution in packings of frictional spheres. Additionally, the effect of particle size ratio and contribution of particle size fractions on energy dissipation in granular mixtures was investigated. The particle size ratio in binary packings was chosen to prevent small particles from percolating through bedding. The bimodality of mixtures was found to have a strong effect on distribution of contact normal orientation and distribution of normal contact forces in binary mixtures. Stress transfer in binary packing was also determined by both, particle size ratio and volume fraction of small particles. Dissipation of energy was higher in mixtures with higher particle size ratios and decreased with increasing contribution of small spheres in system.     

Size determination of diesel soot particles using flow and sedimentation field-flow fractionation

The applicability of field-flow fractionation (FFF) was investigated for determination of size and size distribution of diesel soot particles. A sample preparation procedure was developed for FFF analysis where soot particles are recovered from filters in an ethanol bath sonicator, and then they are dispersed in water containing 0.05% Triton X-100 and 0.02% NaN(3). Mean diameters obtained from sedimentation FFF (SdFFF) and flow FFF (FlFFF) agree well with each other and are in good agreement with diameters obtained from photon correlation spectroscopy (PCS) and scanning electron microscopy. The relative error was less than 11%. Data show diesel soot particles have broad size distributions ranging from 0.05 up to ～0.5 μm with the mean diameters between 0.1 and 0.2 μm. The use of FlFFF is more convenient as FlFFF fractograms can be converted directly to size distributions, while the conversion of the SdFFF fractogram needs the particle density information. The density needed for SdFFF analysis was obtained by combining the SdFFF retention data with the PCS size data. For samples whose density is known, SdFFF may be more useful as SdFFF provides a wider dynamic range than FlFFF under constant field strength.     

Optical properties of internally mixed ammonium sulfate and soot particles--a study of individual aerosol particles and ambient aerosol populations

Optical parameters of simulated ambient individual ammonium sulfate and soot-mixed particles were calculated using the discrete-dipole approximation method with different model geometries. Knowledge of the mixing state and the approximation by a suited idealized geometry reduces the errors of the optical properties by +/-50% to +/-10%. The influence of the soot content and the mixing state on the optical properties of the total aerosol was estimated. For the total aerosol population, the size distribution and the absolute soot content had the largest influence. The exact geometry of the ammonium sulfate and soot-mixed particles can be neglected.     

Fluorescence from airborne microparticles: dependence on size, concentration of fluorophores, and illumination intensity

We measured fluorescence from spherical water droplets containing tryptophan and from aggregates of bacterial cells and compared these measurements with calculations of fluorescence of dielectric spheres. The measured dependence of fluorescence on size, from both droplets and dry-particle aggregates of bacteria, is proportional to the absorption cross section calculated for homogeneous spheres containing the appropriate percentage of tryptophan. However, as the tryptophan concentration of the water droplets is increased, the measured fluorescence from droplets increases less than predicted, probably because of concentration quenching. We model the dependence of the fluorescence on input intensity by assuming that the average time between fluorescence emission events is the sum of the fluorescence lifetime and the excitation lifetime (the average time it takes for an illuminated molecule to be excited), which we calculated assuming that the intensity inside the particle is uniform. Even though the intensity inside the particles spatially varies, this assumption of uniform intensity still leads to results consistent with the measured intensity dependence.     

SEPARATION AND BEHAVIOR OF NONSPHERICAL PARTICLES IN SEDIMENTATION/STERIC FIELD-FLOW FRACTIONATION

Sedimentation/steric field-flow fractionation (Sd/StFFF) is an elution separation technique capable of measuring the size distribution of 0.3-100 µm spherical and near-spherical particles with advantages including high resolution, fast analysis, and the ready collection of narrow size fractions. In this study we investigate the applicability of Sd/StFFF to various nonspherical particles including the doublets of spheres, rod-shaped glass fibers, compressed latex discs, and quartz particles (BCR 67 and 70) with complex mixed shapes. Some fractionation, retention, and selectivity features of these particles are defined and measured in relationship to those of spheres (latex beads), which are better understood. While the relative behavior of these two particle types depends on many factors, especially the distance of the particle from the Sd/StFFF channel wall, in most cases the nonspherical particles are eluted before spheres of equal volume and they often display higher selectivity than spherical particles. However, when retention of nonspherical particles is compared with that for spheres whose diameter is equal to the particle length, elongated particles (doublets and rods) eluted after the sphere while flattened particles (discs) eluted earlier than spheres, an observation that might assist in shape discrimination by Sd/StFFF. Thus, when latex microspheres are used for calibration to obtain size distribution curves, the diameter obtained for any given subpopulation will be less than the length of rods but greater than the diameter of discs. For complex particles such as the quartz particles, the diameter of a particle provided by classical sedimentation using spherical calibration is less than the equivalent spherical diameter of the particle in question whereas Sd/StFFF yields a diameter somewhat greater than the particle length. Thus, these two techniques will yield size distribution curves displaced from one another along the diameter axis. The difference in diameters can be eliminated by using a diameter correction factor of 2.7, which brings the distribution curves for quartz obtained by these two techniques into concurrence.     

Observation of sooting behavior in single droplets combustion in direct current electric fields under microgravity

Because of ions and electrons in flame, flow is induced around flame in electric filed. It affects combustion phenomena, and the effect has seemed to be significant for droplet combustion in previous study. This study is focused on movement of soot particle in single droplets combustion in direct current electric fields under microgravity in order to obtain some information about flow field around droplet. The large soot particles were observed by high-speed CCD camera, and the soot velocities are measured by PTV method. The single droplets were burned in the center of electrodes, which are two parallel rectangular wire nettings. Distance between electrodes is 50mm and applied voltages between electrodes are from 0kV to 6kV. Fuels tested are n-octane and toluene and the initial droplet diameters are around 0.8mm. All experiments were performed in microgravity in order to eliminate the natural convection. The results shows the velocities of soot particle are mainly in the direction of electric field, and most soot particles move to the cathode but some move to the anode. This indicates some soot particles have some negative charges. The velocities of soot particle increase with increasing in the distance from the droplet in both directions, and the velocity to cathode is larger than that to anode. From these results, the change of electric field and flow field around droplet are discussed.     

Strong force networks in granular mixtures

Using the results of 3D discrete element method simulations we study the force transmission through binary mixtures of sand and silt sized spheres under one-dimensional compression. Three types of contact are categorized depending on the size of the two spheres in contact. The contributions of each contact type to the deviator stress are dependent on the proportion of silt sized spheres. We demonstrate that the magnitude of the deviator stress is solely due to the normal and tangential forces at contacts transmitting normal forces greater than a characteristic normal force, which is generally slightly greater than the average normal force. The maximum packing efficiency was obtained with the mixture of 30 % silt sized spheres and this mixture corresponds to a transition point when there are enough silt sized particles to start to separate the sand sized particles from each other and establish contacts between silt sized spheres that contribute to the deviator stress.     

Size influence on optical absorption property of ultra-fine nickel hollow spheres

Nickel hollow spheres (NHSs) with different diameter have been synthesized by the autocatalytic reduction method. The morphology, particle size distribution and optical absorption property of NHSs were investigated. The optical absorption intensity obviously increases in ultraviolet—near infrared region with the decrease of particle size. While in infrared region, nickel hollow spheres have almost no absorption. After the heat treatment process, the grain sizes of samples become bigger and the absorptances decrease in UV–Vis–NIR region. For smaller particles, the absorption peak in ultraviolet range moves from 375 to 440 nm because of the increase of grain size after heat treatment.     

Sensitivity of the backscattering Mueller matrix to particle shape and thermodynamic phase

The Mueller matrix (M) corresponding to the phase matrix in the backscattering region (scattering angles ranging from 175 degrees to 180 degrees) is investigated for light scattering at a 0.532-microm wavelength by hexagonal ice crystals, ice spheres, and water droplets. For hexagonal ice crystals we assume three aspect ratios (plates, compact columns, and columns). It is shown that the contour patterns of the backscattering Mueller matrix elements other than M11, M44, M14, and M41 depend on particle geometry; M22 and M33 are particularly sensitive to the aspect ratio of ice crystals. The Mueller matrix for spherical ice particles is different from those for nonspherical ice particles. In addition to discriminating between spherical and nonspherical particles, the Mueller matrix may offer some insight as to cloud thermodynamic phase. The contour patterns for large ice spheres with an effective size of 100 microm are substantially different from those associated with small water droplets with an effective size of 4 microm.     

Light scattering and absorption by fractal-like carbonaceous chain aggregates: comparison of theories and experiment

This study compares the optical coefficients of size-selected soot particles measured at a wavelength of 870 nm with those predicted by three theories, namely, Rayleigh-Debye-Gans (RDG) approximation, volume-equivalent Mie theory, and integral equation formulation for scattering (IEFS). Soot particles, produced by a premixed ethene flame, were size-selected using two differential mobility analyzers in series, and their scattering and absorption coefficients were measured with nephelometry and photoacoustic spectroscopy. Scanning electron microscopy and image processing techniques were used for the parameterization of the structural properties of the fractal-like soot aggregates. The aggregate structural parameters were used to evaluate the predictions of the optical coefficients based on the three light-scattering and absorption theories. Our results show that the RDG approximation agrees within 10% with the experimental results and the exact electromagnetic calculations of the IEFS theory. Volume-equivalent Mie theory overpredicts the experimental scattering coefficient by a factor of approximately 3.2. The optical coefficients predicted by the RDG approximation showed pronounced sensitivity to changes in monomer mean diameter, the count median diameter of the aggregates, and the geometric standard deviation of the aggregate number size distribution.     

Method for integrating the absorption cross sections of spheres over wavelength or diameter

The absorption cross sections of spherical particles and droplets must be integrated over frequency or droplet size or both for various applications. Morphology-dependent resonances (MDRs) of the spheres can make evaluation of such integrals difficult because the MDRs can contribute significantly to the integrals even when their linewidths are extremely narrow, especially when the absorption is weak. A method of evaluating these integrals by use of Lorentzian approximations near MDRs is described. Calculated frequency-integrated absorption cross sections illustrate how the method obtains accurate cross sections with far fewer integration points than a method that uses equally spaced points. The method reported here suggests a way to integrate over frequency in more-complicated scattering and emission problems and should also be useful for integrating scattering and absorption by other shapes, e.g., spheroids and cylinders, for which the MDR positions and linewidths can be calculated.     

Application of the Hough transform for the automatic determination of soot aggregate morphology

We report a new method for automated identification and measurement of primary particles within soot aggregates as well as the sizes of the aggregates and discuss its application to high-resolution transmission electron microscope (TEM) images of the aggregates. The image processing algorithm is based on an optimized Hough transform, applied to the external border of the aggregate. This achieves a significant data reduction by decomposing the particle border into fragments, which are assumed to be spheres in the present application, consistent with the known morphology of soot aggregates. Unlike traditional techniques, which are ultimately reliant on manual (human) measurement of a small sample of primary particles from a subset of aggregates, this method gives a direct measurement of the sizes of the aggregates and the size distributions of the primary particles of which they are composed. The current version of the algorithm allows processing of high-resolution TEM images by a conventional laptop computer at a rate of 1-2 ms per aggregate. The results were validated by comparison with manual image processing, and excellent agreement was found.     

Mixing narrow coarse and fine coal fractions – The maximum volume fraction of suspensions

A main objective of coal-water slurry fuel (CWSF) preparation is to achieve maximum loading of coal. In the absence of a strong colloidal attractive force, the maximum loading is determined by the packing density of the particles which in turn is a function of the particle size distribution. In this study, coal fractions of different mean sizes with a narrow distribution were separated by sieving. Mixtures of different mean coarse to fine size ratios were then prepared. For each size ratio, different amounts of coarse particle contents were prepared. With these different mixtures, water was added to produce the CWSF. The maximum volume packing density, φ_max, for each mixture was determined using a rheological vane yield stress technique. The determination of φ_max involving the direct yield stress measurements of extremely high concentration suspensions is an entirely new and accurate approach. It was found that the highest φ_max was obtained when the coarse to fine ratio was ～10 located at a coarse coal content of 70 wt%. This result is consistent with that obtained by theoretical modelling of bimodal mixing of monodisperse size spheres with a size ratio of 10. At lower size ratio, φ_max obtained at the optimum coarse coal content was lower.     

单分散γ-Al_2O_3纳米颗粒制备工艺参数的调控

采用均相沉淀法,在950℃煅烧碱式硫酸铝(Al(SO_4)_x(OH)_y)纳米颗粒2h,制备出单分散的γ-Al_2O_3纳米颗粒。研究了阴离子、浓度和沉淀剂/铝盐摩尔比对Al(SO_4)_x(OH)_y颗粒的形貌、尺寸和分散性的影响。结果表明,Al(SO_4)_x(OH)_y颗粒的最佳制备条件为:二甲胺硼烷(DMAB)作沉淀剂、Al_2(SO_4)_3.18H_2O作铝源、[Al~(3+)]=0.0005mol/L、n(DMAB)/n(Al_2(SO_4)_3·18H_2O)=40。制备出的Al(SO_4)_x(OH)_y具有球形、平均颗粒尺寸为98nm、粒径分布为75~130nm、单分散性的特点;获得了球形、平均颗粒尺寸为90nm、粒径分布范围为50~105nm、单分散的γ-Al_2O_3颗粒。     

Optical absorption by randomly oriented carbon spheroids

The optical properties of carbon spheroids are compared with those of carbon spheres for all size regimes. In general, the absorption cross section/unit volume is increased by axial elongation, particularly away from the resonance region. The results are specific to carbon since the effect of shape change in a given size regime can depend crucially on the value of the refractive index.     

Application of the small-angle approximation to ocean water types

The small-angle approximation to the radiative transport equation is applied to particle suspensions that emulate ocean water. A particle size distribution is constructed from polystyrene and glass spheres with the best available data for particle size distributions in the ocean. A volume scattering function is calculated from the Mie theory for the particles in water and in oil. The refractive-index ratios of particles in water and particles in oil are 1.19 and 1.01, respectively. The ratio 1.19 is comparable to minerals and nonliving diatoms in ocean water, and the ratio 1.01 is comparable to the lower limit for microbes in water. The point-spread functions are measured as a function of optical thickness for both water and oil mixtures and compared with the point-spread functions generated from the small-angle approximation. Our results show that, under conditions that emulate ocean water, the small-angle approximation is valid only for small optical thicknesses. Specifically, the approximation is valid only for optical thicknesses less than 3.     

Mesoporous carbon spheres produced by hydrothermal carbonization from rice husk: Optimization,characterization and hydrogen storage

In this study, carbon spheres were synthesized from rice husk with hydrothermal carbonization method at different temperatures and different reaction times. Surface areas and pore size distributions of carbon spheres were characterized by BET surface area device, sphere morphology by SEM, structural characterization by FTIR-ATR and XRD, and thermal properties and degradation mechanism by DTA/TG. In addition, hydrogen gas adsorption measurements of the samples were also carried out with the Hiden IMI PSI gas storage device. It can be said that the required temperature is 280 °C and the required reaction time is 6 h in order to obtain homogeneous and ideal sphere morphology carbon spheres from a lignocellulosic biomass in experiments carried out under different conditions in an acidic reaction medium. This is clearly seen from the SEM images. In addition, FTIR spectra and XRD patterns confirm that the sphere was obtained. According to the BET surface area and pore size distribution results, it can be said that the main significant difference is in the mesopore structure of the carbon spheres, even if the surface area values of the samples obtained at different temperatures and different reaction times increase linearly with temperature. In order to determine the usability of carbon spheres obtained in different conditions in the energy field, the gravimetrically measured H₂ storage capacities at cryogenic temperature (77 K) and pressure range of 0–30 bar were determined as maximum 1.1% by weight. When the hydrogen storage capacities of the samples are evaluated together with the BET surface area values and pore size distributions, it shows that the hydrogen storage capacity in carbon spheres is directly proportional to the mesopore volumes. In addition, Langmuir and Freundlich isotherms related to adsorption equilibrium were investigated in order to better define the H₂ adsorption that took place in these samples. Considering the regression coefficients of the obtained isotherms, it was determined that some of the carbon spheres were more compatible with the Langmuir isotherm and some with the Freundlich isotherm.     

Ice-crystal absorption: a comparison between theory and implications for remote sensing

The problem of the disagreement between cirrus crystal sizes determined remotely and by in situ measurements is shown to be due to inappropriate application of Mie theory. We retrieved the absorption optical depth at 8.3 and 11.1 mum from 11 tropical anvil cirrus clouds, using data from the High Resolution Infrared Radiation Sounder (HIRS). We related the absorption optical depth ratio between the two wavelengths to crystal size (the size was defined in terms of the crystal median mass dimension) by assuming Mie theory applied to ice spheres and anomalous diffraction theory (ADT) applied to hexagonal columns, hexagonal plates, bullet rosettes, and aggregates (polycrystals). The application of Mie theory to retrievals yielded crystal sizes approximately one third those obtained with ADT. The retrievals of crystal size by use of HIRS data are compared with measurements of habit and crystal size obtained from in situ measurements of tropical anvil cirrus particles. The results of the comparison show that ADT provides the more realistic retrieval. Moreover, we demonstrate that at infrared wavelengths retrieval of crystal size depends on assumed habit. The reason why Mie theory predicts smaller sizes than ADT is shown to result from particle geometry and enhanced absorption owing to the capture of photons from above the edge of the particle (tunneling). The contribution of particle geometry to absorption is three times greater than from tunneling, but this process enhances absorption by a further 35%. The complex angular momentum and T-matrix methods are used to show that the contribution to absorption by tunneling is diminished as the asphericity of spheroidal particles is increased. At an aspect ratio of 6 the contribution to the absorption that is due to tunneling is substantially reduced for oblate particles, whereas for prolate particles the tunneling contribution is reduced by 50% relative to the sphere.