The single scattering properties of the aerosol particles as aggregated spheres

The light scattering and absorption properties of anthropogenic aerosol particles such as soot aggregates are complicated in the temporal and spatial distribution, which introduce uncertainty of radiative forcing on global climate change. In order to study the single scattering properties of anthorpogenic aerosol particles, the structures of these aerosols such as soot paticles and soot-containing mixtures with the sulfate or organic matter, are simulated using the parallel diffusion limited aggregation algorithm (DLA) based on the transmission electron microscope images (TEM). Then, the single scattering properties of randomly oriented aerosols, such as scattering matrix, single scattering albedo (SSA), and asymmetry parameter (AP), are computed using the superposition T-matrix method. The comparisons of the single scattering properties of these specific types of clusters with different morphological and chemical factors such as fractal parameters, aspect ratio, monomer radius, mixture mode and refractive index, indicate that these different impact factors can respectively generate the significant influences on the single scattering properties of these aerosols. The results show that aspect ratio of circumscribed shape has relatively small effect on single scattering properties, for both differences of SSA and AP are less than 0.1. However, mixture modes of soot clusters with larger sulfate particles have remarkably important effects on the scattering and absorption properties of aggregated spheres, and SSA of those soot-containing mixtures are increased in proportion to the ratio of larger weakly absorbing attachments. Therefore, these complex aerosols come from man made pollution cannot be neglected in the aerosol retrievals. The study of the single scattering properties on these kinds of aggregated spheres is important and helpful in remote sensing observations and atmospheric radiation balance computations.     

In-flame soot particle structure on the up- and down-swirl side of a wall-interacting jet in a small-bore diesel engine

This study shows how the structure of soot particles within the flame changes due to the relative direction of the swirl flow in a small-bore diesel engine in which significant flame–wall interactions cause about half of the flame travelling against the swirl flow while the other half penetrating in the same direction. The thermophoresis-based particle sampling method was used to collect soot from three different in-flame locations including the flame–wall impingement point near the jet axis and the two 60° off-axis locations on the up-swirl and down-swirl side of the wall-interacting jet. The sampled soot particle images were obtained using transmission electron microscopes and the image post-processing was conducted for statistical analysis of size distribution of soot primary particles and aggregates, fractal dimension, and sub-nanoscale parameters such as the carbon layer fringe length, tortuosity, and spacing. The results show that the jet-wall impingement region is dominated by many small immature particles with amorphous internal structure, which is very different to large, fractal-like soot aggregates sampled from 60° downstream location on the down-swirl side. This structure variation suggests that the small immature particles underwent surface growth, coagulation and aggregation as they travelled along the piston-bowl wall. During this soot growth, the particle internal structure exhibits the transformation from amorphous carbon segments to a typical core–shell structure. Compared to those on the down-swirl side, the soot particles sampled on the up-swirl side show much lower number counts and more compact aggregates composed of highly concentrated primary particles. This soot aggregate structure, together with much narrower carbon layer gap, indicates higher level of soot oxidation on the up-swirl side of the jet.     

Evaluation method for radiative heat transfer in polydisperse water droplets

Simplifications of the model for nongray radiative heat transfer analysis in participating media comprised of polydisperse water droplets are presented. Databases of the radiative properties for a water droplet over a wide range of wavelengths and diameters are constructed using rigorous Mie theory. The accuracy of the radiative properties obtained from the database interpolation is validated by comparing them with those obtained from the Mie calculations. The radiative properties of polydisperse water droplets are compared with those of monodisperse water droplets with equivalent mean diameters. Nongray radiative heat transfer in the anisotropic scattering fog layer, including direct and diffuse solar irradiations and infrared sky flux, is analyzed using REM². The radiative heat fluxes within the fog layer containing polydisperse water droplets are compared with those in the layer containing monodisperse water droplets. Through numerical simulation of the radiative heat transfer, polydisperse water droplets can be approximated by using the Sauter diameter, a technique that can be useful in several research fields, such as engineering and atmospheric science. Although this approximation is valid in the case of pure radiative transfer problems, the Sauter diameter is reconfirmed to be the appropriate diameter for approximating problems in radiative heat transfer, although volume-length mean diameter shows better accordance in some cases. The CPU time for nongray radiative heat transfer analysis with a fog model is evaluated. It is proved that the CPU time is decreased by using the databases and the approximation method for polydisperse particulate media.     

Synchronous measurements of the atmospheric radio emission in the two and three millimeter wavelength regions

Apparatus and procedure of measuring the atmospheric radio emission simultaneously in two atmospheric windows are described. The results of measurements of the sky brightness temperature and obtained atmospheric optical depth values are reported. The diurnal and seasonal variations of the sky temperature and zenith absorption as well as their relation to weather parameters of nearsurface atmospheric layer are discussed.     

Understanding in-cylinder soot reduction in the use of high pressure fuel injection in a small-bore diesel engine

This study shows how soot particles inside the cylinder of the engine are reduced due to high pressure fuel injection used in a light-duty single-cylinder optical diesel engine fuelled with methyl decanoate, a selected surrogate fuel for the diagnostics. For various injection pressures, planar laser induced incandescence (PLII) imaging and planar laser-induced fluorescence of hydroxyl (OH-PLIF) imaging were performed to understand the temporal and spatial development of soot and high-temperature flames. In addition, a thermophoresis-based particle sampling technique was used to obtain transmission electron microscope (TEM) images of soot aggregates and primary particles for detailed morphology analysis. The OH-PLIF images suggest that an increase in the injection pressure leads to wider distribution of high-temperature flames likely due to better mixing. The enhanced high-temperature reaction can promote soot formation evidenced by both a faster increase of LII signals and larger soot aggregates on the TEM images. However, the increased OH radicals at higher injection pressure accelerates the soot oxidation as shown in a higher decreasing rate of LII signals as well as dramatic reduction of the sampled soot aggregates at later crank angles. The analysis of nanoscale carbon layer fringe structures also shows a consistent trend that, at higher injection pressure, the soot particles are more oxidized to form more graphitic carbon layer structures. Therefore, it is concluded that the in-cylinder soot reduction at higher injection pressure conditions is due to enhanced soot oxidation despite increased soot formation.     

针对测量仪器设计的天空亮度分析

天空亮度分布在大气光学领域有着重要的应用。利用Modtran计算了在各种大气、地表条件下的天空亮度分布,分析了大气模式、能见度、云对天空亮度分布的影响,给出了天空亮度的大致动态范围,为天空亮度测量仪器的研制,特别是探测器的选择提供了科学依据。     

Numerical investigation of the effect of signal trapping on soot measurements using LII in laminar coflow diffusion flames

Laser-induced incandescence has been rapidly developed into a powerful diagnostic technique for measurements of soot in many applications. The incandescence intensity generated by laser-heated soot particles at the measurement location suffers the signal trapping effect caused by absorption and scattering by soot particles present between the measurement location and the detector. The signal trapping effect was numerically investigated in soot measurements using both a 2D LII setup and the corresponding point LII setup at detection wavelengths of 400 and 780 nm in a laminar coflow ethylene/air flame. The radiative properties of aggregated soot particles were calculated using the Rayleigh–Debye–Gans polydisperse fractal aggregate theory. The radiative transfer equation in emitting, absorbing, and scattering media was solved using the discrete-ordinates method. The radiation intensity along an arbitrary direction was obtained using the infinitely small weight technique. The contribution of scattering to signal trapping was found to be negligible in atmospheric laminar diffusion flames. When uncorrected LII intensities are used to determine soot particle temperature and the soot volume fraction, the errors are smaller in 2D LII setup where soot particles are excited by a laser sheet. The simple Beer–Lambert exponential attenuation relationship holds in LII applications to axisymmetric flames as long as the effective extinction coefficient is adequately defined.     

Physical-mathematical model of condensation process of the sub-micron dust capture in sprayer scrubber

A physical-mathematical model of the heat and mass exchange process and condensation capture of sub-micron dust particles on the droplets of dispersed liquid in a sprayer scrubber is proposed and analysed. A satisfactory agreement of computed results and experimental data on soot capturing from the cracking gases is obtained.     

一种改进的光谱图像反演地表目标遥感反射率的方法

提出一种改进的反演地表目标遥感反射率的方法．利用光谱图像中的太阳耀光估计当时气象条件下的大气透过率,分析了天空辐射和色散现象对反演的影响,据此构建遥感反演模型,计算出地表目标的遥感反射率．由于消除了天空漫射辐射带来的额外影响使得可见光波段的反演准确度大为提高,此外将菲涅尔反射率表示为波长的函数进行计算使反演光谱在整个波段范围内能更好地匹配实验室光谱．实验结果表明,改进算法计算的反射率能更好地匹配实验室光谱,具有更高的反演准确度．     

Cellular pattern formation in detonation propagation

The relation between the soot track on smoked plate records and the frontal structure of gaseous detonations was experimentally studied to clarify the mechanism of cellular pattern formation by using combination images of high-speed schlieren pictures, self-emission images of the reaction front, and the smoked plate record. Several materials were tested as alternatives to soot particles of smoked foil technique to record detonation structure. The experimental results show that the triple point trajectory coincides with the soot track and that cellular cell-like patterns are obtained for CaCO₃ particles, fly ash, heat-sensitive paper, and pressure-sensitive paper. An asymmetrical cellular pattern in the smoked plate record is exhibited in the case of the pressure-sensitive paper, while a symmetrical pattern is observed for the other materials. This asymmetry is successfully explained by the temporal response of the pressure-sensitive paper from evaluation of time integration of pressure, namely impulse to time varying loading. Estimation of wall shear stress and tensile strength of agglomerated particles layer on the basis of an analogy to particle entrainment from fine powder layers shows the critical particle diameter for removal of particles. However, the shear stress is found to be not strong enough for removal of particles located in the triple point trajectory. Finally other additional mechanisms for local detachment of particles are discussed.     

In situ, real-time detection of soot particles coated with NaCl using 193 nm light

We report in situ, real-time detection of soot particles coated with NaCl using excimer laser fragmentation fluorescence spectroscopy (ELFFS). Carbon atom fluorescence at 248 nm and the Na D-line at 589 nm are used as signatures of soot and NaCl, respectively. Soot particles are encapsulated with a NaCl layer in a well-controlled inverted flame burner. NaCl particles are injected into the methane-air co-flow flame to coat the soot particles. ArF laser irradiation of the coated particles in an air stream at 1.14 J/cm² produces fluorescence from Na, C, and CH. At 0.69 J/cm², which is slightly above the fluorescence threshold, but not enough for considerable fragmentation of the particles, Na D-line persists with little carbon and no CH observed. These results suggest that the photolytic fragmentation-fluorescence using 193 nm excitation can be effectively used for in situ, real-time chemical analysis of core-shell nanoparticles. PACS 78.67.Bf; 78.70.-g; 42.68.Jg     

Surface deposition and coagulation efficiency of combustion generated nanoparticles in the size range from 1 to 10 nm

The size distribution of the nanoparticles formed in premixed ethylene–air flames and collected thermophoretically on mica cleaved substrates is obtained by atomic force microscopy (AFM). The distribution function extends from 1 to about 5 nm in non-sooting flames and in the soot pre-inception region of the richer flames, while it becomes bimodal and larger particles are formed in the soot inception region of the slightly sooting flames. The distribution is compared with the size distribution of nano-sized organic carbon (NOC) and soot particles, obtained by “in situ” multi-wavelength extinction and light scattering methods. The deposition efficiency is estimated from the differences between these two size distribution functions as a function of the equivalent diameter of the nanoparticles. Furthermore, the coagulation coefficient of particles in flame is obtained from the temporal evolution of the number concentration of the nanoparticles inside the flames. NOC particles, which are rapidly produced in locally rich combustion regions, have peculiar properties since their sticking coefficient both for coagulation and adhesion result to be orders of magnitudes lower than that expected by larger aerosols, like soot particles. The experimental results are interpreted by modelling the van der Waals interactions of the nanoparticles in terms of Lennard-Jones potentials and in the framework of the gas kinetic theory. The estimated adhesion and coagulation efficiencies are in good agreement with those calculated from AFM and optical data. The very low efficiency values observed for the smaller particles could be ascribed to the high energy of these particles due to their Brownian motion, which causes thermal rebound effects prevailing over adhesion mechanisms due to van der Waals forces.     

一种改进的光谱图像反演地表目标遥感反射率的方法

提出一种改进的反演地表目标遥感反射率的方法.利用光谱图像中的太阳耀光估计当时气象条件下的大气透过率,分析了天空辐射和色散现象对反演的影响,据此构建遥感反演模型,计算出地表目标的遥感反射率.由于消除了天空漫射辐射带来的额外影响使得可见光波段的反演准确度大为提高,此外将菲涅尔反射率表示为波长的函数进行计算使反演光谱在整个波段范围内能更好地匹配实验室光谱.实验结果表明,改进算法计算的反射率能更好地匹配实验室光谱,具有更高的反演准确度.     

The effect of particle aggregation on the absorption and emission properties of mono- and polydisperse soot aggregates

This study concerns the effect of soot-particle aggregation on the soot temperature derived from the signal ratio in two-color laser-induced incandescence measurements. The emissivity of aggregated fractal soot particles was calculated using both the commonly used Rayleigh–Debye–Gans fractal-aggregate theory and the generalized Mie-solution method in conjunction with numerically generated fractal aggregates of specified fractal parameters typical of flame-generated soot. The effect of aggregation on soot temperature was first evaluated for monodisperse aggregates of different sizes and for a lognormally distributed aggregate ensemble at given signal ratios between the two wavelengths. Numerical calculations were also conducted to account for the effect of aggregation on both laser heating and thermal emission at the two wavelengths for determining the effective soot temperature of polydisperse soot aggregates. The results show that the effect of aggregation on laser energy absorption is important at low fluences. The effect of aggregation on soot emissivity is relatively unimportant in LII applications to typical laminar diffusion flames at atmospheric pressure, but it can become more important in flames at high pressures due to larger primary particles and wider aggregate distributions associated with enhanced soot loading.     

Influence of pressure on near nozzle flow field and soot formation in laminar co-flow diffusion flames

Soot formation from combustion devices, which tend to operate at high pressure, is a health and environmental concern, thus investigating the effect of pressure on soot formation is important. While most fundamental studies have utilised the co-flow laminar diffusion flame configuration to study the effect of pressure on soot, there is a lack of investigations into the effect of pressure on the flow field of diffusion flames and the resultant influence on soot formation. A recent work has displayed that recirculation zones can form along the centreline of atmospheric pressure diffusion flames. This present work seeks to investigate whether these zones can form due to higher pressure as well, which has never been explored experimentally or numerically. The CoFlame code, which models co-flow laminar, sooting, diffusion flames, is validated for the prediction of recirculation zones using experimental flow field data for a set of atmospheric pressure flames. The code is subsequently utilised to model ethane-air diffusion flames from 2 to 33 atm. Above 10 atm, recirculation zones are predicted to form. The reason for the formation of the zones is determined to be due to increasing shear between the air and fuel steams, with the air stream having higher velocities in the vicinity of the fuel tube tip than the fuel stream. This increase in shear is shown to be the cause of the recirculation zones formed in previously investigated atmospheric flames as well. Finally, the recirculation zone is determined as a probable cause of the experimentally observed formation of a large mass of soot covering the entire fuel tube exit for an ethane diffusion flame at 36.5 atm. Previously, no adequate explanation for the formation of the large mass of soot existed.     

The Formation of Carbon in Combustion and how to Quantify the Impact on Human Health

We summarize our current research on combustion aerosols. First, sampling devices for the analyses of flame gases are described. The flame gas samples are investigated by mass spectroscopy and by standard aerosol techniques. Time-of-flight mass spectroscopy is well suited to study formation and growth of soot precursor molecules. Fullerenes can also be seen in some mass spectra of flame gases. Presumably, the fullerenes are evaporated from small soot particles in the mass spectrometer by the ionizing laser. Size spectra of soot particles from the flame are presented. The flame is optionally seeded with palladium aerosol to demonstrate that the particle size distribution is not altered during the sampling procedure. It is found that soot particles are already present low in the flame where large molecules are absent.Photoemission is applied to study surface properties of soot particles from the flame. It is shown that the surface of the particles is covered with polycyclic aromatic hydrocarbons (PAH). The PAH can be removed by heating and the properties of the carbon core are revealed. One can thereby distinguish a soot growth from a soot burnout region in the flame. Time-resolved desorption experiments of perylene (a PAH) from model aerosol particles are presented. It is shown that they follow a first order rate law. The photoelectric PAH sensor is introduced as a personal air quality monitor. The danger from inhaling combustion aerosol can be expressed in units of standard cigarettes.     

Effect of soot shape on soot radiation

It is increasingly recognized that soot particles play an important role in the radiative heat transfer from flames and smoke. After their formation, these minute particles usually conglomerate into different forms, with the limiting shapes being the spheres and long chains which can be modeled as infinite cylinders. The present work analyzes the effect of soot shape on soot radiation. The spectral extinction coefficient of spheres, being lower than that of the cylindrical particles, falls off rapidly in the near i.r. The shape effect on soot radiation is found to be more pronounced at low temperatures than at high temperatures. In flame radiation calculations the radiative contribution of the various conglomerated soot shapes can be properly accounted for by assuming spherical and polydisperse soot particles. Based on the extinction characteristics of the particles, an experimental method for determining the amount of spherical and cylindrical particles in a soot cloud is suggested.     

团簇状碳黑颗粒在丙烯臭氧氧化和光氧化体系中的重构

大气中的碳黑颗粒具有不规则的分形团簇结构. 以电火花放电产生的团簇碳黑颗粒为研究对象,发现颗粒的团簇结构在丙烯臭氧氧化和光氧化体系中均发生重构,形成更为紧实的结构. 研究表明这种重构是由丙烯氧化产生的过氧自由基和羟基自由基引起的. 研究结果有助于对大气中团簇状碳黑颗粒老化过程的进一步了解. 由于重构直接改变了颗粒的粒径分布,这一过程可能导致碳黑颗粒在大气中物理化学特性的重大改变. 关键词： 团簇碳黑颗粒 重构 丙烯 烟雾箱     

Soot particles in piston-top pool fires and exhaust at 5 and 15 MPa injection pressure in a gasoline direct-injection engine

This study shows the structure of soot particles sampled directly from wall wetting-induced pool fires formed on the piston top in a spark-ignition direct-injection (SIDI) engine. Of particular interest is its variation with injection pressure considering the current trend of high-pressure DI system development to reduce engine-out particulate emissions. Thermophoretic particle sampling was performed for transmission electron microscope (TEM) imaging, which was post-processed for statistical analysis of key morphology and internal structure parameters. These include the size distribution of soot aggregates and primary particles as well as carbon-layer fringe-to-fringe gap and concentricity. With the fixed engine speed and load conditions, in-flame soot particles are compared to the exhaust particles sampled simultaneously at selected 5 and 15 MPa injection pressures corresponding to low-speed/low-load and high-speed/high-load in practical engine operation. From the TEM images and statistical analysis, it was found that more concentrated and taller pool fire developed for 5-MPa injection leads to smaller soot aggregates composed of smaller soot primary particles due to suppressed soot growth in fuel-rich flames. However, the soot particles formed in 15-MPa injection-induced pool fires are at a more reactive status evidenced by less defined core-shell boundaries and higher fringe separation. The higher soot reactivity results in enhanced soot oxidation, which explains smaller soot aggregates and primary particles found for the 15-MPa injection in the exhaust sample.     

Influence of polydisperse distributions of both primary particle and aggregate size on soot temperature in low-fluence LII

An improved aggregate-based low-fluence laser-induced incandescence (LII) model has been developed. The shielding effect in heat conduction between aggregated soot particles and the surrounding gas was modeled using the concept of the equivalent heat transfer sphere. The diameter of such an equivalent sphere was determined from direct simulation Monte Carlo calculations in the free molecular regime as functions of the aggregate size and the thermal accommodation coefficient of soot. Both the primary soot particle diameter and the aggregate size distributions are assumed to be lognormal. The effective temperature of a soot particle ensemble containing different primary particle diameters and aggregate sizes in the laser probe volume was calculated based on the ratio of the total thermal radiation intensities of soot particles at 400 and 780 nm to simulate the experimentally measured soot particle temperature using two-color optical pyrometry. The effect of primary particle diameter polydispersity is in general important and should be considered. The effect of aggregate size polydispersity is relatively unimportant when the heat conduction between the primary particles and the surrounding gas takes place in the free-molecular regime; however, it starts to become important when the heat conduction process occurs in the near transition regime. The model developed in this study was also applied to the re-determination of the thermal accommodation coefficient of soot in an atmospheric pressure laminar ethylene diffusion flame. PACS 44.05.+e; 61.46.Df; 65.80.+n