High-vacuum time-resolved laser-induced incandescence of flame-generated soot

We have measured time-resolved laser-induced incandescence of flame-generated soot under high-vacuum conditions (4.1×10⁻⁶ mbar) at an excitation wavelength of 532 nm with laser fluences spanning 0.06–0.5 J/cm². We generated soot in an ethylene/air diffusion flame, introduced it into the vacuum system with an aerodynamic lens, heated it using a pulsed laser with a spatially homogeneous and temporally smooth laser profile, and recorded LII temporal profiles at 685 nm. At low laser fluences LII signal decay rates are slow, and LII signals persist beyond the residence time of the soot particles in the detection region. At these fluences, the temporal maximum of the LII signal increases nearly linearly with increasing laser fluence until reaching a plateau at ∼0.18 J/cm². At higher fluences, the LII signal maximum is independent of laser fluence within experimental uncertainty. At these fluences, the LII signal decays rapidly during the laser pulse. The fluence dependence of the vacuum LII signal is qualitatively similar to that observed under similar laser conditions in an atmospheric flame but requires higher fluences (by ∼0.03 J/cm²) for initiation. These data demonstrate the feasibility of recording vacuum LII temporal profiles of flame-generated soot under well-characterized conditions for model validation.     

Experimental and theoretical comparison of spatially resolved laser-induced incandescence (LII) signals of soot in backward and right-angle configuration

In-situ measurements of soot volume fraction in the exhausts of jet engines can be carried out using the laser-induced incandescence (LII) technique in backward configuration, in which the signal is detected in the opposite direction of the laser beam propagation. In order to improve backward LII for quantitative measurements, we have in this work made a detailed experimental and theoretical investigation in which backward LII has been compared with the more commonly used right-angle LII technique. Both configurations were used in simultaneous visualization experiments at various pulse energies and gate timings in a stabilized methane diffusion flame. The spatial near-Gaussian laser energy distribution was monitored on-line as well as the time-resolved LII signal. A heat and mass transfer model for soot particles exposed to laser radiation was used to theoretically predict both the temporal and spatial LII signals. Comparison between experimental and theoretical LII signals indicates similar general behaviour, for example the broadening of the spatial LII distribution and the hole-burning effect at centre of the beam due to sublimation for increasing laser pulse energies. However, our comparison also indicates that the current heat and mass transfer model overpredicts signal intensities at higher fluence, and possible reasons for this behaviour are discussed. PACS 42.62.Fi; 44.40.+a     

Laser-induced incandescence for soot particle size and volume fraction measurements using on-line extinction calibration

A novel technique for two-dimensional measurements of soot volume fraction and particle size has been developed. It is based on a combined measurement of extinction and laser-induced incandescence using Nd:YAG laser wavelengths of 532 nm and 1064 nm. A low-energy laser pulse at 532 nm was used for extinction measurements and was followed by a more intense pulse at 1064 nm, delayed by 15 ns, for LII measurements. The 532-nm beam was split into a signal beam passing the flame and a reference beam, both of which were directed to a dye cell. The resulting fluorescence signals, from which the extinction was deduced, together with the LII signal, were registered on a single CCD detector. Thus the two-dimensional LII image could be converted to a soot volume fraction map through a calibration procedure during the same laser shot. The soot particle sizes were evaluated from the ratio of the temporal LII signals at two gate time positions. The uncertainty in the particle sizing arose mainly from the low signal for small particles at long gate times and the uncertainty in the flame temperature. The technique was applied to a well-characterized premixed flat flame, the soot properties of which had been previously thoroughly investigated. Received: 21 June 2000 / Revised version: 11 September 2000 / Published online: 7 February 2001     

LII–lidar: range-resolved backward picosecond laser-induced incandescence

A novel concept for remote in situ detection of soot emissions by a combination of laser-induced incandescence (LII) and light detection and ranging (lidar) is presented. A lidar setup based on a picosecond Nd:YAG laser and time-resolved signal detection in the backward direction was used for LII measurements in sooty premixed ethylene–air flames. Measurements of LII–lidar signal versus laser fluence and flame equivalence ratio showed good qualitative agreement with data reported in literature. The LII–lidar signal showed a decay consisting of two components, with lifetimes of typically 20 and 70 ns, attributed to soot sublimation and conductive cooling, respectively. Theoretical considerations and analysis of the LII–lidar signal showed that the derivative was proportional to the maximum value, which is an established measure of soot volume fraction. Utilizing this, differentiation of LII–lidar data gave profiles representing soot volume fraction with a range resolution of ~16 cm along the laser beam propagation axis. The accuracy of the evaluated LII-profiles was confirmed by comparison with LII-data measured simultaneously employing conventional right-angle detection. Thus, LII–lidar provides range-resolved single-ended detection, resourceful when optical access is restricted, extending the LII technique and opening up new possibilities for laser-based diagnostics of soot and other carbonaceous particles.     

Influence of the cumulative effects of multiple laser pulses on laser-induced incandescence signals from soot

The effect of multiple laser pulses reaching soot particles before an actual laser-induced incandescence (LII) measurement is investigated in order to gain some insights on soot morphological and fine structure changes due to rapid laser heating. Soot, extracted from a premixed and a quenched diffusion flames, is flowing through a tubular cell and undergoes a variable number of pulses at different fluence. The response of soot is studied by the two-color LII technique. Transmission electron microscopy (TEM) analysis of laser-modified soot aggregates from the diffusion flame is also presented. The results indicate that even at low laser fluences a permanent soot transformation is induced causing an increase in the absorption function E(m). This is interpreted as an induced graphitization of soot particles by the laser pulse heating. At high fluences the vaporization process and a profound restructuring of soot particles affect the morphology of the aggregates. Soot from diffusion and premixed flames behaves in a similar way although this similarity occurs at different fluence levels indicating a different initial fine structure of soot particles.     

Laser-induced incandescence of flame-generated soot on a picosecond time scale

This paper presents measurements of time-resolved laser-induced incandescence (LII) from soot recorded on a picosecond time scale. The 532-nm output from a picosecond Nd:YAG laser was used to heat the soot, and a streak camera was used to record the LII signal. The results are compared with data collected on a nanosecond time scale and with a time-dependent model that solves the energy- and mass-balance rate equations. Relative to the laser timing, the picosecond and nanosecond results are very similar. Signals increase during the laser pulse as soot temperatures increase and decrease after the laser pulse. The signal decay rates increase significantly with increasing laser fluence. The LII model gives good agreement with the nanosecond data at fluences ≤0.2 J/cm² and underpredicts the signal decay rates at higher fluences. The picosecond temporal profiles increase significantly faster and earlier in the laser pulse than predicted by the model. This disagreement between the model and picosecond LII data may be attributable to perturbations to the signal by laser-induced fluorescence from polycyclic aromatic hydrocarbons or other large organic species. The excited state or states responsible for this fluorescence appear to be accessed via a two-photon transition and have an effective lifetime of 55 ps. PACS 44.40.+a; 78.67.Bf; 78.47.+p     

Effects of volatile coatings on the laser-induced incandescence of soot

We have measured time-resolved laser-induced incandescence (LII) from combustion-generated mature soot extracted from a burner and (1) coated with oleic acid or (2) coated with oleic acid and then thermally denuded using a thermodenuder. The soot samples were size selected using a differential mobility analyzer and characterized with a scanning mobility particle sizer, centrifugal particle mass analyzer, and transmission electron microscope. The results demonstrate a strong influence of coatings on the magnitude and temporal evolution of the LII signal. For coated particles, higher laser fluences are required to reach signal levels comparable to those of uncoated particles. The peak LII curve is shifted to increasingly higher fluences with increasing coating thickness until this effect saturates at a coating thickness of ~75 % by mass. These effects are predominantly attributable to the additional energy needed to vaporize the coating while heating the particle. LII signals are higher and signal decay rates are significantly slower for thermally denuded particles relative to coated or uncoated particles, particularly at low and intermediate laser fluences. Our results suggest negligible coating enhancement in absorption cross-section for combustion-generated soot at the laser fluences used. Apparent enhancement in absorption with restructuring may be caused by less conductive cooling.     

Relationship between soot volume fraction and LII signal in AC-LII: effect of primary soot particle diameter polydispersity

Theoretical analysis and numerical calculations were conducted to investigate the relationship between soot volume fraction and laser-induced incandescence (LII) signal within the context of the auto-compensating LII technique. The emphasis of this study lies in the effect of primary soot particle diameter polydispersity. The LII model was solved for a wide range of primary soot particle diameters from 2 to 80 nm. For a log-normally distributed soot particle ensemble encountered in a typical laminar diffusion flame at atmospheric pressure, the LII signals at 400 and 780 nm were calculated. To quantify the effects of sublimation and differential conduction cooling on the determined soot volume fraction in auto-compensating LII, two new quantities were introduced and demonstrated to be useful in LII study: an emission intensity distribution function and a scaled soot volume fraction. When the laser fluence is sufficiently low to avoid soot mass loss due to sublimation, accurate soot volume fraction can be obtained as long as the LII signals are detected within the first 200 ns after the onset of the laser pulse. When the laser fluence is in the high fluence regime to induce significant sublimation, however, the LII signals should be detected as early as possible even before the laser pulse reaches its peak when the laser fluence is sufficiently high. The analysis method is shown to be useful to provide guidance for soot volume fraction measurements using the auto-compensating LII technique.     

Investigation on the influence of soot size on prompt LII signals in flames

Theoretical papers predict that prompt LII signals are weakly dependent on the soot size due to the fact that larger particles reach higher temperatures during the heating process by nanosecond laser pulses. This question is of crucial importance for establishing LII as a practical technique for soot volume fraction measurements. In this work two-color prompt LII measurements have been performed in several locations of diffusion and rich premixed ethylene-air flames. The experimental apparatus was carefully designed with a probe volume of uniform light distribution and sharp edges, a 4 ns integration time around the signal pulse peak and narrow spectral bandwidth. Measurements did not confirm the theoretical predictions concerning an increase of temperature for larger particles. On the contrary, larger particles in richer premixed flames exhibit a lower 400/700 signal ratio. This can probably be attributed to small differences in the refractive index of soot.     

Influence of spatial laser energy distribution on evaluated soot particle sizes using two-colour laser-induced incandescence in a flat premixed ethylene/air flame

Time-resolved laser-induced incandescence (LII) has been developed rapidly during the last decade as a useful non-intrusive technique for particle size determination. Still several parameters should be investigated in order to improve the accuracy of LII for particle sizing and the spatial distribution of the laser energy is one of these. Generally a top-hat profile is recommended, as this ensures a uniform heating of all particles in the measurement volume. As it is generally not straightforward to create a uniform beam profile, it is of interest to establish the influence of various profiles on the evaluated particle sizes. In this work we present both an experimental and a theoretical investigation of the influence of the spatial profile on evaluated sizes. All experiments were carried out using a newly developed setup for two-colour LII (2C-LII) which provides online monitoring of both the spatial and temporal profile as well as the laser pulse energy. The LII measurements were performed in a one-dimensional premixed sooting ethylene/air flame, and evaluated particle sizes from LII were compared with thermophoretically sampled soot particles analysed using transmission electron microscopy (TEM). The results show that although there is some influence of the spatial laser energy distribution on the evaluated particle sizes both in modelling and experiments, this effect is substantially smaller than the influence of the uncertainties in gas temperature and the thermal accommodation coefficient.     

The effects of pulsed laser injection seeding and triggering on the temporal behavior and magnitude of laser-induced incandescence from soot

The effect of sub-nanosecond fluence fluctuations and triggering on time-resolved laser-induced incandescence (LII) from soot has been studied using an injection-seeded pulsed Nd:YAG laser that produces a smooth laser temporal profile. Without injection seeding, this multi-mode laser generates pulses with large intensity fluctuations with sub-nanosecond rise times. The experimental results described here demonstrate that at fluences below 0.6 J/cm² LII signals are insensitive to fluence fluctuations on nanosecond time scales. At fluences above 0.6 J/cm² fluctuations in the laser profile cause the rising edge of the LII profile to move around in time relative to the center of the laser pulse causing a broader average profile that shifts to earlier times. Such fluctuations also lead to a decrease in the average LII temporal profile by up to 12% at a fluence of 3.5 J/cm². A timing jitter on the trigger of the data acquisition, such as that produced by triggering on the laser Q-switch synchronization pulse, has a negligible effect on the shape and temporal maximum of the LII signal. Additional jitter, however, considerably reduces the peak of the LII temporal profiles at fluences as low as 0.15 J/cm². Neither fast fluence fluctuations nor trigger jitter have a significant effect on gated LII signals, such as those used to infer soot volume fraction.     

Soot sublimation studies in a premixed flat flame using laser-induced incandescence (LII) and elastic light scattering (ELS)

Laser-induced incandescence (LII) as a diagnostic technique is based on rapid heating of soot particles to temperatures of several thousand Kelvin and subsequent detection of the thermal radiation from the laser-heated particles. At such high temperatures, soot sublimation effects must be considered when estimating uncertainties in LII measurements. In this work we have investigated the use of various laser fluences in LII using a Nd:YAG laser at 1,064 nm. Using another Nd:YAG laser at 532 nm, the elastic light scattering (ELS) signal from soot particles heated by the 1,064-nm laser was monitored. This approach makes it possible to determine at which fluence of the LII laser soot sublimation starts to become visible as a decrease in the ELS signal. By performing the measurements at various heights in a premixed sooting flat ethylene/air flame, the fluence threshold above which the ELS signal decreased was found to be higher at the lower flame heights corresponding to younger, smaller and less aggregated particles. The results from this work indicate that the different fluence thresholds for sublimation may be explained by a lower absorption function E(m) for the younger soot particles.     

Soot formation characteristics in a lab-scale turbulent pulverized coal flame with simultaneous planar measurements of laser induced incandescence of soot and Mie scattering of pulverized coal

Soot formation characteristics of a lab-scale pulverized coal flame were investigated by performing carefully controlled laser diagnostics. The spatial distributions of soot volume fraction and the pulverized coal particles were measured simultaneously by laser induced incandescence (LII) and Mie scattering imaging, respectively. In addition, the radial distributions of the soot volume fraction were compared with the OH radical fluorescence, gas temperature and oxygen concentration obtained in our previous studies [1], [2]. The results indicated that the laser pulse fluence used for LII measurement should be carefully controlled to measure the soot volume fraction in pulverized coal flames. To precisely measure the soot volume fraction in pulverized coal flames using LII, it is necessary to adjust the laser pulse fluence so that it is sufficiently high to heat up all the soot particles to the sublimation temperature but also sufficiently low to avoid including a too large of a change in the morphology of the soot particles and the superposition of the LII signal from the pulverized coal particles on that from the soot particles. It was also found that the radial position of the peak LII signal intensity was located between the positions of the peak Mie scattering signal intensity and peak OH radical signal intensity. The region, in which LII signal, OH radical fluorescence and Mie scattering coexisted, expanded with increasing height above the burner port. It was also found that the soot formation in pulverized coal flames was enhanced at locations where the conditions of high temperature, low oxygen concentration and the existence of pulverized coal particles were satisfied simultaneously.     

Optical and microscopy investigations of soot structure alterations by laser-induced incandescence

2 at 1064 nm, vaporization/fragmentation of soot primary particles and aggregates occurs. Optical measurements are performed using a second laser pulse to probe the effects of these changes upon the LII signal. With the exception of very low fluences, the structural changes induced in the soot lead to a decreased LII intensity produced by the second laser pulse. These two-pulse experiments also show that these changes do not alter the LII signal on timescales less than 1 μs for fluences below the vaporization threshold. Received: 20 October 1997/Revised version: 16 February 1998     

Simultaneous planar measurements of soot structure and velocity fields in a turbulent lifted jet flame at 3 kHz

We describe a newly developed combustion diagnostic for the simultaneous planar imaging of soot structure and velocity fields in a highly sooting, lifted turbulent jet flame at 3000 frames per second, or two orders of magnitude faster than “conventional” laser imaging systems. This diagnostic uses short pulse duration (8 ns), frequency-doubled, diode-pumped solid state (DPSS) lasers to excite laser-induced incandescence (LII) at 3 kHz, which is then imaged onto a high framerate CMOS camera. A second (dual-cavity) DPSS laser and CMOS camera form the basis of a particle image velocity (PIV) system used to acquire 2-component velocity field in the flame. The LII response curve (measured in a laminar propane diffusion flame) is presented and the combined diagnostics then applied in a heavily sooting lifted turbulent jet flame. The potential challenges and rewards of application of this combined imaging technique at high speeds are discussed.     

Investigation on thermal accommodation coefficient and soot absorption function with two-color Tire-LII technique in rich premixed flames

Although the two-color laser-induced incandescence technique (2C-LII) has proved to be a significant tool for soot diagnostics, many efforts are still required to gain a whole understanding of the chemical and physical processes involved. Time-resolved two-color LII measurements are carried out in a rich ethylene/air premixed flame at different heights above the burner and by changing the laser fluence. The prompt LII at two wavelengths and the corresponding soot incandescence temperature are obtained at different stages of the soot growth and under different laser irradiations. The decay rate of the LII signals, as a method for soot sizing, is investigated at different laser fluence. The time-resolved LII curves, obtained in the low laser fluence regime, are analyzed by a numerical simulation, available on the web. By considering the gas/particle initial temperature obtained with thermocouple measurements and by knowing soot particle diameter with previous TEM and extinction/scattering measurements, information about soot parameters, such as absorption function and thermal accommodation coefficient are obtained. The presence of the so-called young or mature soot along the flame height is strictly related to different optical and heat-exchange properties necessary to fit all the experimental data available.     

The concept of 2D gated imaging for particle sizing in a laminar diffusion flame

In this work, time-resolved laser-induced incandescence (TiRe LII) has been employed to measure primary particle diameters of soot in an atmospheric laminar ethylene diffusion flame. The generated data set complements existing data determined in one single location and takes advantage of the good spatial resolution of the ICCD detection. Time resolution is achieved by shifting the camera gate along the LII decay. One key input parameter for the analysis of time-resolved LII is the local flame temperature. This was determined on a grid throughout the flame by coherent anti-Stokes Raman scattering. The accurate temperature data, in combination with other published data from this flame, are well suited for soot model validation purposes while we showed feasibility of a shifted gate approach to deduce 2D particle sizes in the chosen standard flame.     

Constraints of two-colour TiRe-LII at elevated pressures

The main objective of this work is to investigate the influence of high-pressure conditions on the determination of primary particle size distributions of laser-heated soot particles using pyrometrically determined temperature decays. The method is based on time-resolved laser-induced incandescence measurements carried out at two different wavelengths (two-colour TiRe-LII). The LII signals are transferred into a particle ensemble averaged (effective) temperature using Planck’s thermal radiation formula. Assuming that all particles within the size distribution possess a unique temperature at the end of the laser pulse, the size distribution can be determined by numerically simulating the measured temperature decay. From our investigations, for pressures up to a few bars it is obvious that this strategy can be successfully applied if standard laser pulses of nano-second duration are used as an LII-excitation source. At higher pressures the time scales of heat conduction are decreased to such an extent that a unique temperature for all particles within the ensemble cannot be assumed at the end of the nano-second laser pulse. However, further investigations show that the presented two-colour TiRe-LII technique can be successfully adopted under technical high-pressure conditions as well, if the pulse duration of the TiRe-LII-excitation source is reduced into the pico-second range.     

Comparison of LII derived soot temperature measurements with LII model predictions for soot in a laminar diffusion flame

Laser-induced incandescence (LII) was used to derive temperatures of pulsed laser heated soot particles from their thermal emission intensities detected at two wavelengths in a laminar ethylene/air co-annular diffusion flame. The results are compared to those of a numerical nanoscale heat and mass transfer model. Both aggregate and primary particle soot size distributions were measured using transmission electron microscopy (TEM). The model predictions were numerically averaged over these experimentally derived size distributions. The excitation laser wavelength was 532 nm, and the LII signal was detected at 445 nm and 780 nm. A wide range of laser fluence from very low to moderate (0.13 to 1.56 mJ/mm²) was used in the experiments. A large part of the temporal decay curve, beginning 12–15 nsec after the peak of the laser excitation pulse, is successfully described by the model, resulting in the determination of accommodation coefficients, which varies somewhat with soot temperature and is in the range of 0.36 to 0.46. However, in the soot evaporative regime, the model greatly overpredicts the cooling rate shortly after the laser pulse. At lower fluences, where evaporation is negligible, the initial experimental cooling rates, immediately following the laser pulse, are anomalously high. Potential physical processes that could account for these effects are discussed. From the present data the soot absorption function, E(m), of 0.4 at 532 nm is obtained. A procedure for correcting the measured signals for the flame radiation is presented. It is further shown that accounting for the local gas temperature increase due to heat transfer from soot particles to the gas significantly improves the agreement in the temperature dependence of soot cooling rates between model and experiments over a large range of laser fluences.     

Laser-induced incandescence for soot-particle sizing at elevated pressure

This paper describes the applicability of laser-induced incandescence (LII) as a measurement technique for primary soot particle sizes at elevated pressure. A high-pressure burner was constructed that provides stable, laminar, sooting, premixed ethylene/air flames at 1–10 bar. An LII model was set up that includes different heat-conduction sub-models and used an accommodation coefficient of 0.25 for all pressures studied. Based on this model experimental time-resolved LII signals recorded at different positions in the flame were evaluated with respect to the mean particle diameter of a log-normal particle-size distribution. The resulting primary particle sizes were compared to results from TEM images of soot samples that were collected thermophoretically from the high-pressure flame. The LII results are in good agreement with the mean primary particle sizes of a log-normal particle-size distribution obtained from the TEM-data for all pressures, if the LII signals are evaluated with the heat-conduction model of Fuchs combined with an aggregate sub-model that describes the reduced heat conduction of aggregated primary soot particles. The model, called LIISim, is available online via a web interface. PACS 65.80.+n; 78.20.Nv; 42.62.-b; 47.70.Pq