Quantitative experimental measurements of soot concentrations and soot scattering are presented for a series of steady and flickering coflowing methane, propane, and ethylene flames burning at atmospheric pressure. Flickering diffusion flames exhibit a wide range of time-dependent, vortex-flame sheet interactions, and thus they serve as an important testing ground for assessing the applicability of chemical models derived from steady flames. Acoustic forcing of the fuel flow rate is used to phase lock the periodic flame flicker close to the natural flame flicker frequency caused by buoyancy-induced instabilities. For conditions in which flame clip-off occurs, the peak soot concentrations in the methane flickering flames are 5.5 to 6 times larger than measured in a steady flame burning with the same mean fuel flow rate, whereas the enhancement for the flickering propane and ethylene flames is only 35 to 60%, independent of the flicker intensity. Soot concentration profiles and full Mie analysis of the soot volume fraction/scattering results reveal significant differences in the structure of the soot fields and in the roles of soot inception, growth, and oxidation for the different hydrocarbon fuels. The soot concentrations have been measured using laser-induced incandescence (LII). Since this is the only technique currently available for making time- and spatially-resolved soot concentration measurements in time-varying flow fields, considerable effort has been devoted to developing LII for quantitative applications. Important considerations include (1) proper calibration measurements, (2) signal detection which minimizes interferences from C2 Swan-band emission and broadband molecular fluorescence, (3) correction for the laser beam focus/spatial averaging effect in line image measurements, and (4) correction for LII signal extinction within the flame.

An in situ particulate diagnostic/analysis technique is outlined based on the Rayleigh-Debye-Gans polydisperse fractal aggregate (RDG/PFA) scattering interpretation of absolute angular light scattering and extinction measurements. Using proper particle refractive index, the proposed data analysis method can quantitatively yield all aggregate parameters (particle volume fraction, fv, fractal dimension, Df, primary particle diameter, dp, particle number density, np, and aggregate size distribution, pdf(N)) without any prior knowledge about the particle-laden environment. The present optical diagnostic/interpretation technique was applied to two different soot-containing laminar and turbulent ethylene/air nonpremixed flames in order to assess its reliability. The aggregate interpretation of optical measurements yielded Df, dp, and pdf(N) that are in excellent agreement with ex situ thermophoretic sampling/transmission electron microscope (TS/TEM) observations within experimental uncertainties. However, volume-equivalent single particle models (Rayleigh/Mie) overestimated dp by about a factor of 3, causing an order of magnitude underestimation in np. Consequently, soot surface areas and growth rates were in error by a factor of 3, emphasizing that aggregation effects need to be taken into account when using optical diagnostics for a reliable understanding of soot formation/evolution mechanism in flames. The results also indicated that total soot emissivities were generally underestimated using Rayleigh analysis (up to 50%), mainly due to the uncertainties in soot refractive indices at infrared wavelengths. This suggests that aggregate considerations may not be essential for reasonable radiation heat transfer predictions from luminous flames because of fortuitous error cancellation, resulting in typically a 10 to 30% net effect.

Simultaneous measurements of laser-induced incandescence (LII) and elastic scattering from soot particles in diesel engine exhaust have been made. The LII signal scaled linearly with the mass concentration of the non-volatile particulate mass fraction over the entire range of engine operating loads. Over this range of conditions, the volume mean diameter of the soot particles varied from 0.07 to 0.11 mu m, but the size change did not appear to affect the signal response. The scattering response did not scale linearly with the mass concentration of soot. Mass concentrations of 0.2 mg/m3 were easily detectable, with even lower values possible. Additional techniques for determining the volatile fraction of particulate mass are described. (Author abstract). EiPLUS (c) 1996 Engineering Information Inc.

The spectral extinction coefficients of soot aggregates were studied in the fuel-lean (overfire) region of buoyant turbulent diffusion flames. Extinction measurements were carried out in the wavelength region of 0.2-5.2 mu m for flames fueled with acetylene, propylene, ethylene, and propane, burning in air. The present measurements were combined with earlier measurements of soot morphology and light scattering at 0.514 mu m in order to evaluate the spectral soot refractive indices reported by Dalzell and Sarofim (1969), Lee and Tien (1981), and Chang and Charalampopoulos (1990). The specific extinction coefficients and emissivities were predicted based on Rayleigh-Debye-Gans theory for polydisperse fractal aggregates, which has been recently found to be the best approximation to treat optical cross sections of soot aggregates. The results indicated that available refractive indices of soot do not predict the spectral trends of present measurements in the ultraviolet and infrared regions. Soot complex refractive index was inferred to be m = 1.54 + 0.48i at 0.514 mu m, which is surprisingly in best agreement with the values reported by Dalzell and Sarofim (1969). Additionally, specific extinction coefficients of soot aggregates varied with wavelength as lambda(-0.83) from the visible to the infrared. Finally soot refractive indices were found to be relatively independent of fuel type for the visible and infrared spectral regions over the H/C ratio range of 0.08-0.22.

The structure of soot aggregates was investigated, emphasizing the fractal properties as well as the relationships between the properties of actual and projected soot images. This information was developed by considering numerically simulated soot aggregates based on cluster-cluster aggregation as well as measured soot aggregates based on thermophoretic sampling and analysis by transmission electron microscopy (TEM) of soot for a variety of fuels (acetylene, propylene, ethylene, and propane) and both laminar and turbulent diffusion flame conditions. It was found that soot aggregate fractal properties are relatively independent of fuel type and flame condition, yielding a fractal dimension of 1.82 and a fractal prefactor of 8.5, with experimental uncertainties (95% confidence) of 0.08 and 0.5, respectively. Relationships between the actual and projected structure properties of soot, e.g., between the number of primary particles and the projected area and between the radius of gyration of an aggregate and its projected image, also are relatively independent of fuel type and flame condition.

A recently developed laser-induced incandescence technique is used to make novel planar measurements of soot volume fraction within turbulent diffusion flames and droplet flames. The two-dimensional imaging technique is developed and assessed by systematic experiments in a coannular laminar diffusion flame, in which the soot characteristics have been well established. With a single point calibration procedure, agreement to within 10% was found between the values of soot volume fraction measured by this technique and those determined by conventional laser scattering-extinction methods in the flame. As a demonstration of the wide range of applicability of the technique, soot volume fraction images are also obtained from both turbulent ethene diffusion flames and from a freely falling droplet flame that burns the mixture of 75% benzene and 25% methanol. For the turbulent diffusion flames, approximately an 80% reduction in soot volume fraction was found when the Reynolds number of the fuel jet increased from 4000 to 8000. In the droplet flame case, the distribution of soot field was found to be similar to that observed in coannular laminar diffusion flames.

Optical cross-sections of carbonaceous aggregates (smoke) formed by combustion sources have been computed based on fractal concepts. Specific extinction depends upon the primary particle size, the structure of the aggregates as represented by the fractal dimension, the fractal prefactor, and the real and imaginary components of the refractive index of the particle material. While the fractal dimension and primary particle diam. are narrowly defined, the refractive index, to which the results are highly sensitive, are disputed. Specific extinction was measured at .lambda. = 450, 630, and 1000 nm in a smoke-filled chamber with an optical path length of 1.0 m that was equipped to continuously monitor both particle mass and no. concn. as the smoke aged during a 90-120 min interval. The smoke was generated by the burning of crude oil in a pool fire. Specific extinction at all three values of .lambda. was const. even though the aggregate no. concn. decreases by a factor of 24 owing to cluster-cluster aggregation. The refractive indexes at several wavelengths that are required to give agreement with the measured specific extinction are compared with literature values. The inadequacy of Mie theory for spheres in predicting the optical properties of soot aggregates is reiterated.

Laser-Induced Incandescence (LII) occurs when a high-energy pulsed laser is used to heat soot to incandescent temperatures. Theoretical calculations predict and experimental tests demonstrate the resulting incandescence to be a measure of soot-volume fraction. Practical implementation of the technique is detailed by examining the spectral character, temporal behavior, and excitation-intensity dependence of the resulting thermal emission from the laser-heated soot in both premixed and diffusion flames. Spatial and temporal capabilities of LII are demonstrated by obtaining one- and two-dimensional images of soot-volume fraction via laser-induced incandescence in both types of flames.

Laser-induced incandescence is used to obtain spatially resolved measurements of soot volume fraction in a laminar diffusion flame, excellent agreement. In addition, the laser-induced incandescence signal is observed to involve a rapid rise in intensity followed by a relatively long (ca. 600 ns) decay period subsequent to the laser pulse, while the effect of laser fluence is manifest in nonlinear and near-saturated response of the laser-induced incandescence signal. Laser-induced incandescence can be used as an instantaneous, spatially resolved diagnostic of soot volume fraction without the need for the conventional line-of-sight laser extinction method, while potential applications in two-dimensional imaging and simultaneous measurements of laser-induced incandescence and light-scattering to generate a complete soot property characterization are significant. (Edited author abstract).