Laser-induced Incandescence Measurements Research Articles

Role of the Equivalence Ratio on Soot Formation in a Perfectly Premixed Turbulent Swirled Flame: A Combined Experimental and Large Eddy Simulations Study

Abstract The understanding of processes that govern soot production in aero-engines is fundamental for the design of new combustion systems with low environmental impact. Many combustors, more specifically those used in aero-engines, feature rich flame regions typically exploited in the so-called rich-quench-lean (RQL) technology. Thus, it is important to consider rich turbulent flames operating in the premixed mode. To this purpose, a model scale swirled combustor, called EM2Soot, was designed at the EM2C laboratory to analyze soot production under perfectly premixed rich conditions. In this work, the effect of the equivalence ratio on soot production in this burner is experimentally characterized and numerically simulated. Measurements of Planar Laser Induced Fluorescence of polycyclic aromatic hydrocarbons (PLIF-PAH) were performed to examine soot precursors presence, whereas soot volume fraction is measured with planar laser-induced incandescence (LII). Large Eddy Simulations (LES) are carried out using models already established in literature. By considering a range of equivalence ratios, the soot volume fraction from the experiments was found to reach a maximum near 1.8, whereas a lower level of soot volume fraction was measured for lower and for higher equivalence ratios. The large eddy simulations are found to be in qualitative agreement with experimental data in terms of polycyclic aromatic hydrocarbons (PAHs) and soot location. The soot volume fractions fv are notably overestimated with respect to the LII measurements. However, the numerical results correctly retrieve a reduction of soot production for the highest considered equivalence ratio value and can be used to explain the experimental behavior.

A Comprehensive Review of Optical Systems for Soot Volume Fraction Measurements in Co-Flow Laminar Flames: Laser-Induced Incandescence (LII) and Laser Extinction Method (LEM)

ABSTRACT Laser-Induced Incandescence (LII) has been widely acknowledged as a highly effective method for measuring soot in co-flow laminar flames. Conversely, quantitative assessments of soot volume fraction (SVF) are achievable through the Laser Extinction Method (LEM). This comprehensive review centers on the optical systems and experimental parameter configurations employed in LII and LEM measurements. Subsequently, several pivotal parameters specific to LII and LEM, such as laser fluence and detection wavelength, are individually discussed. Furthermore, this review showcases current experimental arrangements utilized for LEM measurements. In addition, recommendations are provided for the execution of planar LII and LEM measurements. Lastly, a summarized analysis and discussion pertain to an optical system capable of jointly measuring LII and LEM.

Numerical and experimental investigations on the particle formation in oxymethylene ethers (OME[formula omitted], n = 2−4)/ethylene premixed flames

Alternative synthetic fuels can be produced by renewable energy sources and represent a potential route for solving long-term energy storage. Among them, oxygenated fuels have the advantage of significantly reducing pollutant emissions and can therefore be used as carbon-neutral substitute fuels for transportation. In this work, the sooting propensity of different oxymethylene ethers (OMEs) is investigated using a combined experimental and numerical study on a series of burner-stabilized premixed flames under mild to severe sooting conditions. Herein, mixtures of ethylene in combination with the three individual oxymethylene ether (OMEn) for n=2,3,4 are compared in terms of soot formation behavior with pure ethylene flames. The kinetic mechanism from Sun et al. (Proc. Combust. Inst. 36 (2017) 1269–1278) for OMEn combustion with n=1,2,3 is extended to include OME4 decomposition and combustion kinetics. It is combined with a detailed quadvariate soot model, which uses the Conditional Quadrature Method of Moments (CQMOM), and the soot simulation results are validated with Laser-Induced Fluorescence (LIF) and Laser-Induced Incandescence (LII) measurements. It is observed that the three investigated OMEn with n=2,3,4 show similar sooting behavior, mainly reducing larger aggregates while not significantly affecting the formation of smaller particles. Furthermore, the extent of soot reduction is comparable among the three OMEn. The trends and overall reduction are captured very well by the model. The modeling results are analyzed through reaction pathway analyses and sensitivity studies that show the importance of OMEn decomposition and the formation of formaldehyde (CH2O) under rich conditions for reducing species relevant for soot precursor formation. These findings are based on the negligible differences in soot formation between the different OMEn fuels observed in this study.

Initial interpretation of Laser-induced Incandescence (LII) signals from flame-generated TiO2 particles: Towards a quantitative characterization of the flame synthesis processes

Among various optical diagnostics for the characterization of particle formation in flames, laser-induced incandescence (LII), developed for soot particles, is attracting attention for the study of flame synthesis of metal-oxides. Among them, TiO2 nanoparticles are widely used for pigments and photocatalysts. Recent works have shown the feasibility of LII for flame-synthesized TiO2, but extensive research is still needed to quantitatively characterize TiO2 production in flames with LII measurements. In this work, the first attempt towards the characterization of TiO2 synthesis in flames is provided as a normalized volume fraction. To achieve this, TiO2 nanoparticles are generated in a laminar coflow diffusion flame of argon-diluted hydrogen and air with pre-vaporized titanium isopropoxide (TTIP). A 355 nm laser is used to irradiate the flame-generated particles. Spectral, temporal, and spatial measurements are performed at various flame heights. First, laser-induced emission (LIE) at prompt is investigated for different laser fluences to identify the operating conditions that ensure the LII-like nature of the measured signals. The LIE at high fluence presents sharp features that contain information on the atomic composition of the particles and of the vaporized species when compared to reference spectra of carbon black and high-purity TiO2 particles. Then, the LII signal at lower fluence is used to obtain an estimation of the spatial evolution of the normalized volume fraction and of the LII signal decay time. These results are finally used to discuss the major aerosol processes along the flame centerline.

Laser irradiation of differently aged carbon nanoparticles: effect on optical properties

The effect of laser irradiation on carbon nanoparticles of different maturity sampled from a premixed flame is investigated. To this purpose, extinction and laser-induced incandescence measurements are carried out on pristine and pre-irradiated nanoparticles. From extinction measurements, a spectral trend of the absorption coefficient of the particles is retrieved. Moreover, two-color laser-induced incandescence versus fluence is used to investigate the behavior of signal and temperature fluence curves in the different conditions under analysis. By coupling these results, interesting outcomes are obtained depending on the nature (nascent vs mature) of the particles. For nascent particles, a significant shift of the fluence curves is observed for the pre-irradiated particles, suggesting an increase in the absorption efficiency. However, no changes in the spectral trend of the absorption coefficient are observed from extinction measurements. On the contrary, for mature particles the absorption properties are strongly affected by irradiation resulting in an increase in the absorption efficiency in the spectral region below 600 nm. Moreover, a decrease of the temperature at the plateau regime for pre-irradiated mature particles towards the temperature value reached by nascent particles is observed. Two processes, namely fragmentation and sublimation followed by nucleation of new particles are suggested to occur under laser irradiation, especially for mature carbon nanoparticles.

Spectral investigation of soot absorption properties during laser-induced incandescence measurements

The effect of rapid laser irradiation on the optical properties of mature soot particles is investigated by performing wavelength-resolved extinction measurements in the visible spectral region. In particular, the spectral behavior of the absorption properties is explored during laser irradiation, at the peak of the incandescence signal (prompt LII) and few nanoseconds after the peak, and finally when particles have reached an equilibrium condition with the surrounding gas. A significant variation of the absorption coefficient of the laser-irradiated soot particles compared to that of the pristine ones is observed already at the LII peak. Such variation keeps evolving with time until it reaches a final permanent value. Results are presented in relation to the laser fluence used for irradiation and discussed with the aim of stressing the need of knowing the entity of the modification of soot absorption properties during laser irradiation for a correct interpretation of LII data.

Time-resolved laser-induced incandescence on metal nanoparticles: effect of nanoparticle aggregation and sintering

This work examines the excessive absorption and anomalous cooling phenomena reported in laser-induced incandescence measurements on metal nanoparticles by considering the effects of aggregate structure and sintering. Experimental investigations are conducted on iron and molybdenum aerosols, which have different melting points, and thus respond differently to the laser pulse. Although aggregation enhances the absorption cross-section of the nanoparticles and allows for higher peak temperatures, this enhancement does not fully explain the observed excessive absorption. Furthermore, as the aggregates of refractory metals such as molybdenum cool, they may sinter through gradual grain boundary diffusion; this change in structure alters their absorption cross-section, manifesting as a rapid drop in the pyrometric temperature, which could explain the anomalous cooling reported for this metal.

Laser diagnostics to characterize the in-flame growth of platinum nanoparticles manufactured by the reactive spray deposition technology

Reactive Spray Deposition Technology (RSDT) is an atmospheric pressure, flame-based advanced manufacturing method used to fabricate Membrane Electrode Assemblies (MEAs) for proton exchange fuel cells and water electrolyzers. RSDT combines the flame synthesis of catalyst nanoparticles and their deposition onto the membrane in one step. The properties of the synthesized nanoparticles, such as their Size Distribution Function (SDF), determine the manufactured electrodes’ performance, which can be evaluated when the deposition is complete via ex-situ characterization of the products. Efforts to improve RSDT for manufacturing state-of-the-art MEAs can be significantly enhanced with integrated laser diagnostics that enable in situ measurement of the synthesized catalyst nanoparticles. This paper reports the implementation of laser diagnostics in an RSDT facility and evaluates their potential to assist the manufacturing process. Laser Light Scattering (LS) and Laser-Induced Incandescence (LII) measurements are performed in the oxygen-rich zone of the flame at various distances from the flame fuel jet nozzle downstream of its luminous region. The measurements quantitatively track the evolution in size and volume fraction of platinum-based nanoparticles in two flames that yield different catalytic properties in the manufactured electrodes. The profiles of the measured nanoparticles’ volume fraction along the flame axis can be estimated a priori so that the average nanoparticle sizes can be measured in quasi-real time via LS. Nanoparticles experience an extremely slow growth rate while being convected at distances from 150 nm to 300 nm from the fuel nozzle. Complementary characterizations of the synthesized nanoparticles are performed ex-situ via High-Angle Annular Darkfield Scanning Transmission Electron Microscopy (HAADF-STEM) image analyses of samples collected on grids at a fixed distance from the fuel jet nozzle. Comparing the results from laser and microscopy techniques not only cross-validates the findings but also provides the parameters to infer the bimodal SDF in-situ and yields evidence that the coagulation efficiency of the synthesized nanoparticles has extremely low values in the investigated zone of the flames.

Parameterization of a Refined Model Aimed at Simulating Laser-Induced Incandescence of Soot Using a Visible Excitation Wavelength of 532 nm

Laser-induced incandescence (LII) is one of the most powerful techniques for soot detection in combustion media. It is therefore commonly used to perform experiments in lab-scale flames and industrial combustors with a view to elucidating the formation mechanisms leading to combustion-generated fine carbonaceous particles while assessing their intrinsic properties. Quantitatively interpreting LII measurements, however, requires a firm knowledge of the optical properties of soot, including their wavelength-dependent absorption function (). Among the approaches used to evaluate such a crucial parameter, one can implement a LII model to derive the value which has to be set to reproduce a series of LII signals measured in a well-characterized environment. In this context, the present work aims at parameterizing a refined LII model built upon a comprehensive version of soot heat- and mass-balance equations for assessment when using a visible excitation wavelength of 532 nm. The proposed model integrates terms representing the saturation of linear, single- and multi-photon absorption processes, cooling by sublimation, conduction, radiation and thermionic emission, in addition to mechanisms depicting soot oxidation and annealing, non-thermal photodesorption of carbon clusters, as well as corrective factors accounting for the shielding effect and multiple scattering (MS) within aggregates. To parameterize this advanced simulation tool, an optimization procedure coupling design of experiments with a genetic algorithm-based solver was implemented. Doing so allowed to estimate the values of different factors involved in absorption and sublimation terms, including the multi-photon absorption cross-section for C2 photodesorption, the saturation coefficients for linear- and multi-photon absorption, as well as the value. Obtained parameters turned out to be well-suited to reproduce a set of LII signals acquired in a Diesel flame. While leading to predictions merging on a single curve with measured data, the so-parameterized model notably led to infer values of 0.3 and 0.38 when considering or neglecting MS within aggregates, respectively. Finally, the / ratio estimated based on data collected herein and in a former modeling work was found to be consistent with results issued from two-excitation wavelength LII measurements previously reported in the literature.

Influence of rapid laser heating on differently matured soot with double-pulse laser-induced incandescence

For accurate laser-induced incandescence (LII) measurements of soot properties it is of great importance to understand the nature of the physical processes involved during rapid laser heating. In this work, we investigate how well-characterized differently matured fresh soot from a soot generator responds to rapid laser heating. For this purpose, a double-pulse LII setup is used with 10 μs time separation between the pulses using various combinations of two common LII wavelengths (532 and 1064 nm). Detection is performed at two wavelength bands for fluorescence analysis, and additionally elastic light scattering is used for mass loss analysis during heating. We investigate how the LII signal changes with pre-heating laser energy, specifically by fluence curve analysis to estimate the influence of thermal annealing, sublimation and laser-induced fluorescence interference. It is shown that extensive absorption enhancement occurs for all types of soot as the soot is thermally annealed, which is manifested through decreasing dispersion coefficient ξ and an increasing absorption coefficient E(m,λ). When comparing young and mature soot, a much larger impact of sublimation can be observed in the fluence curves of the mature soot. Also, we observe an enhanced contribution of laser-induced fluorescence for the young soot when performing LII measurements using 532 nm, which is suggested to originate from vaporized carbon fragments with an aromatic structure. This work further shows the potential of utilizing double-pulse arrangements for increasing the detectability of poorly absorbing soot, but also it highlights the impact of laser heating on soot, which may be important to avoid interferences when performing soot diagnostics.

Laser-induced incandescence for non-soot nanoparticles: recent trends and current challenges

Laser-induced incandescence (LII) is a widely used combustion diagnostic for in situ measurements of soot primary particle sizes and volume fractions in flames, exhaust gases, and the atmosphere. Increasingly, however, it is applied to characterize engineered nanomaterials, driven by the increasing industrial relevance of these materials and the fundamental scientific insights that may be obtained from these measurements. This review describes the state of the art as well as open research challenges and new opportunities that arise from LII measurements on non-soot nanoparticles. An overview of the basic LII model, along with statistical techniques for inferring quantities-of-interest and associated uncertainties is provided, with a review of the application of LII to various classes of materials, including elemental particles, oxide and nitride materials, and non-soot carbonaceous materials, and core–shell particles. The paper concludes with a discussion of combined and complementary diagnostics, and an outlook of future research.

A layer-peeling method for signal trapping correction in planar LII measurements of statistically steady flames

This work presents a layer-peeling (LP) algorithm to correct the signal trapping effect in planar laser-induced incandescence (LII) measurements of soot volume fraction. The method is based on measurements of LII signals captured by an intensified CCD camera at a series of parallel planes across a diffusion flame. A method based on presumed function (PF) of soot volume fraction is also proposed for comparison. The presented methods are numerically tested based on synthetic LII signals emitted from a simulated axisymmetric laminar diffusion flame using the CoFlame code. Numerical results showed that the LP method is able to correct the signal trapping effect, even for fairly large optical thicknesses and in a wide range of detection wavelengths. The correction decreases the relative errors induced by neglecting the trapping effect considerably. The signal trapping effect correction is less important for the determination of integrated soot quantities such as radially integrated soot volume fraction or total soot loading. Planar LII measurements were carried out and calibrated in order to test the method experimentally in a coflow flame. The LP, PF and a simplified analytical (SA) model were compared. The results indicate that the differences in soot volume fraction of 1 ppm or about 15% are obtained in zones of maximum soot loading of 6.5 ppm when the trapping effect is accounted for. Also, the LP and SA methods were found computationally efficient and accurate compared to the PF method. Although the study was performed in a canonical laminar axisymmetric flame, the proposed method can be applied to any statistically steady 3D flame.

Planar Light Extinction Measurement of Soot Volume Fraction in Laminar Counterflow Diffusion Flames

A cost-effective and straightforward light extinction method has been extensively used for measurement of soot volume fraction (SVF) in sooting flames. The traditional pointwise measurement with translation stage suffers from relatively time-consuming operation and low spatial resolution. In the current study, the planar light extinction method is processed by utilizing a CMOS camera to image the combustion field of counterflow diffusion flame (CDF) backlit with the lamp. Collimated and diffuse optical layouts were adopted to explore the feasibility. Investigations of beam-steering effects are presented and discussed through a combination of computational fluid dynamics (CFD) and ray tracing simulations. Measured SVF are compared to the well-validated laser-induced incandescence (LII) measurements. Current measurements show that the diffuse optical layout is feasible and robust to provide accurate and more efficient measurement of the SVF in CDF with superior spatial resolution (21.65 μm).

Time-Resolved Laser-Induced Incandescence Measurements on Aerosolized Nickel Nanoparticles.

This work presents the first quantitative analysis of time-resolved laser-induced incandescence (TiRe-LII) measurements on aerosolized nickel nanoparticles in several gases and over a range of laser fluences. A measurement model composed of spectroscopic and heat transfer submodels is used to recover the particle size distribution parameters and the thermal accommodation coefficient (TAC). A qualitative analysis of the results reveals evidence of nonincandescent laser-induced emission temporally aligned with the laser pulse, and more laser energy is absorbed than can be accounted for from the modeled spectral absorption cross section of the nanoparticles. The TiRe-LII inferred particle size parameters were generally consistent with values found from ex situ transmission electron microscopy (TEM) analysis. The TACs for nickel nanoparticles in polyatomic gases were larger than those in monoatomic gases, which may indicate chemisorption.

Multiphoton induced photoluminescence during time-resolved laser-induced incandescence experiments on silver and gold nanoparticles

In conventional time-resolved laser-induced incandescence (TiRe-LII) measurements, a laser pulse heats the nanoparticles within a probe volume of aerosol, and the particle size distribution and other characteristics are inferred from the observed incandescence decay rate, which is connected to the change in sensible energy through a spectroscopic model. There is strong evidence, however, that for some aerosol systems, the incandescence signal is contaminated with other non-incandescent emission sources. Recent TiRe-LII measurements on polydisperse aerosolized silver and gold nanoparticles energized with a 1064 nm laser pulse exhibit broadband emission that is temporally aligned with the temporal profile of the laser pulse, suggesting that the signal is due to non-thermal emission. One candidate for this emission phenomenon is multiphoton-induced upconversion luminescence, in which the conduction-band electron gas is heated up to an effective lattice temperature, resulting in luminescence due to high-energy intraband transitions.

Laser induced incandescence measurement of soot in ethylene buoyant turbulent diffusion flames under normal and reduced oxygen concentrations

There is a lack of published soot measurement data in buoyant turbulent flames under reduced oxygen conditions. In this work, the laser induced incandescence (LII) technique is used to investigate the soot volume fraction (fv) and soot sheet thickness in buoyant turbulent diffusion flames in atmospheres with different oxygen concentrations (OC, oxygen molar fraction in oxidizer). The experiments establish an extensive database of quantitative fv spatial distribution in ethylene flames under three OCs (20.9%, 16.8%, and 15.2%) and two heat release rates (HRR = 10 kW and 15 kW). Mean, fluctuation, and probability density function of fv, as well as local soot intermittency are studied and compared across different conditions. The results show that the maximum instantaneous fv in normal air can be ~8 ppm; but the corresponding mean fv only reaches up to 0.58 ppm due to turbulence and flame intermittency. As the oxygen concentration is reduced from 20.9% to 15.2%, the mean fv decreases, and this effect is more significant at lower heights above the burner (e.g., ~75% reduction in the mean fv at a height of half a burner outer diameter). Soot is found to be distributed unevenly in the flame, appearing in sheet-like regions with irregular and complicated shapes. The soot sheet thickness is quantified to better understand soot-turbulence interactions. This soot dataset, along with other accompanying radiation and flow field measurements, provides a comprehensive understanding of the dynamics of turbulent buoyant flame dynamics under normal and vitiated conditions, and can be used to develop and validate models for soot formation and radiative heat transfer in such flames.

Effects of pressure on soot production in piloted turbulent non-premixed jet flames

Laser-induced incandescence (LII) was used to quantify the soot volume fraction in five piloted turbulent non-premixed C2H4-N2 jet flames at elevated pressures. In one series of flames, the bulk jet velocity was held constant as the pressure was increased from 1 bar (Re = 10,000) to 3 bar (Re = 30,000), and then 5 bar (Re = 50,000). In the other series, a Reynolds number of 10,000 was held constant at 1 bar, 3 bar, and 5 bar. LII measurements were calibrated with laminar diffusion flames at each pressure using 2D diffuse line-of-sight attenuation. Mean and RMS soot volume fractions along the flame centerline exhibit Gaussian profiles for all of the flames. The magnitude of soot volume fraction and the spatial soot distribution are enhanced by increases in pressure. In both series of flames, the peak mean soot volume fraction scales with the pressure as p2.2. In the constant velocity series, the scaling drops to p1.5 if the volume-integrated mean soot volume fraction on a per fuel mass basis is considered instead. At 3 bar, a threefold increase in Re leads to a decrease in the mean soot volume fraction despite the decrease in soot intermittency. At 5 bar, a fivefold increase in Re results in soot intermittency near zero at the flame’s center and a slight increase in the mean soot volume fraction.

In-flow optical characterization of flame-generated carbon nanoparticles sampled from a premixed flame

In this work, the optical absorption properties of carbon nanoparticles are investigated by applying in-flow extinction and laser-induced incandescence measurements. Carbon nanoparticles are produced in an ethylene/air premixed flame and sampled at different heights above the burner. From extinction measurements, the absorption coefficient is obtained in a wide spectral range, considering the negligible scattering under our experimental conditions. With the application of Tauc plot the optical band gap is evaluated at the sampling heights under analysis. The increase of this value with the decrease in the height is consistent with the quantum confinement effect detected in the inception region of the flame. Two-color laser induced incandescence measurements are performed at relatively high laser fluence. The fluence curves, given by the particle temperature under laser irradiation versus laser fluence, are also obtained. A significant difference in the optical properties of these particles is observed by changing the sampling height. Moreover, considering the fluence curve in the low laser fluence regime, the refractive index absorption function E(m) is evaluated at an excitation wavelength of 1064 nm. Finally, the knowledge of the behavior of the absorption coefficient in a wide spectral range allows retrieving the values and the behavior of E(m) as a function of wavelength.

Impact of Oxygenated Additives on Soot Properties during Diesel Combustion

Emissions from diesel engines can be limited and potentially decreased by modifying the fuel chemical composition through additive insertion. One class of additives that have shown to be particularly efficient in the reduction of the particulates from the combustion of diesel fuels are oxygenated compounds. In the present study we investigate the effect of tripropylene glycol methyl ether (TPGME) and two polyoxymethylene dimethyl ethers (POMDME or OMEs) on soot formation in a laminar diesel diffusion flame. From the evaluation of soot volume fraction by laser-induced incandescence (LII) measurements we could observe that OME additives have a substantial capability (higher compared to TPGME) to decrease the particle concentration, which drops by up to 36% with respect to the pure diesel fuel. We also note a reduction in particle aggregate size, determined by wide-angle light scattering (WALS) measurements, which is more pronounced in the case of OME–diesel blends. The effects we observe can be correlated to the higher amount of oxygen content in the OME molecules. Moreover, both additives investigated seem to have almost no impact on the local soot temperature which could in turn play a key role in the production of soot particles.

Soot maturity studies in methane-air diffusion flames at elevated pressures using laser-induced incandescence

Two-dimensional laser-induced incandescence (LII) measurements were used for quantitative soot volume fraction (fv) measurements in methane-air diffusion flames at pressures ranging from 0.1 to 0.5 MPa. Additionally, laser-induced fluorescence (LIF) was used for visualization of polycyclic aromatic hydrocarbons (PAHs) considered as important soot precursors. A heat and mass transfer-based LII model was used for the analysis of experimental LII fluence curves to evaluate soot absorption functions, E(m), at various spatial positions in the flames. Based on previous work, variations in the evaluated E(m) was assumed to be related to soot maturity. Generally, the most mature soot was found at the spatial position of maximum fv along the central axis and at the flame edges. Also, the soot maturity at the position of maximum fv at each pressure was found to increase from the flame at 0.1 MPa to 0.5 MPa. A critical examination of the assumptions and uncertainties in the E(m) analysis was made. The present study emphasizes the limitation of assigning soot a constant E(m) in the overall flame for temperature and soot concentration evaluation using the optical methods spectral soot emission (SSE) and line-of-sight attenuation (LOSA), which are commonly used non-intrusive optical diagnostic techniques in sooting high-pressure flames. The study also demonstrates the critical choice of fluence in quantitative imaging LII measurements of fv when the E(m) of soot spans over large range of values.