Multi-scalar measurements in a premixed swirl burner using 1D Raman/Rayleigh scattering

Instantaneous measurements of temperature, equivalence ratio, and major species were performed along a one-dimensional probe volume using simultaneous Raman/Rayleigh scattering in an unconfined turbulent lean-premixed swirling methane/air flame. Temperature was determined from Rayleigh scattering and the major species, CO₂, O₂, N₂, CH₄, H₂O, and H₂ from Raman scattering. Effective Rayleigh cross-sections were corrected using the local chemical composition obtained from Raman scattering. These experiments were conducted to investigate the compositional structure of a lean-premixed swirling flame in detail and to complement previous measurements of the underlying flow field. The flame was classified within a revised regime diagram at the cross-over between corrugated flames and thin reaction zones. Instantaneous temperature profiles varied significantly showing shapes ranging from laminar-like flamelets to mixing between reacted fluid elements and secondary air. Different thermo-kinetic states could be assigned to the inner and outer recirculation zones and to the inner and outer mixing layers. Linked to published velocity data of this flame, the present multi-scalar data are useful for validation of numerical simulations.     

Pressure dependence of vibrational Raman scattering of narrow-band, 248-nm, laser light by H2, N2, O2, CO2, CH4, C2H6, and C3H8 as high as 97 bar

We have previously investigated methods that image high-pressure processes such as combustion inside automobile cylinders and aircraft engines, or chemical phenomena in supercritical fluids. Here we show that vibrational Raman scattering can simply obtain, quantitatively, densities of some combustion-relevant molecules. We use narrow-band KrF excimer-laser light. Measurements for H₂, N₂, O₂, CO₂, and CH₄ are in the pressure range from 1 to 60 bar, whereas those for C₂H₆ and C₃H₈ are up to their respective vapor pressures. All these species are at ambient temperature. Additional measurements are described for CO₂ up to 96.8 bar and 318 K, where CO₂ is a supercritical fluid. The O₂ measurements are complicated by a photochemical formation of O₃; those in supercritical CO₂ by drastic bending of the laser beam within this medium. We show that, for each gas, the Raman signal is directly proportional to gas density, thereby making quantitative analysis particularly convenient. For each species, we present an estimate of its Raman cross-section relative to that of N₂. However we recommend that future diagnostics users calibrate their own systems for relative species sensitivity. Received: 23 December 1999 / Revised version: 6 June 2000 / Published online: 20 September 2000     

Tunable,sub-nanosecond KrF-Raman laser in the ultraviolet

A 0.5 cm^–1 bandwidth injection-locked KrF laser pumps a rare-gas Brillouin cell to produce a reflected pulse with a leading edge risetime of 1 ns, tunable from 248.1 to 248.7 nm. Consistent with Lamb theory of laser amplifiers, subsequent excimer amplification of this pulse produces an intense 500 ps spike on the pulse leading edge. Stimulated Raman scattering then separates the spike from the parent pulse, yielding a tunable short pulse at the first Stokes (S ₁) wavelength. Varying the Raman cell length results in a variable Raman threshold and an adjustable short pulse duration: 250 ps pulses at energies of 3–4 mJ at 268 nm with a 50 cm methane cell and 350 ps, 5 mJ pulses from a 100 cm cell are measured with a streak camera. First pass Raman conversion of the spike toS ₁ followed by second pass backward Raman amplification, where the parent 248 nm pulse serves as the pump beam for the reflectedS ₁ pulse, yields simultaneousS ₁ pulses of 20–25 mJ in the 800 ps range andS ₂ pulses of 550 ps at 5–6 mJ near 290 nm. This laser will avoid collision effects during laser excitation and enable quantitative, single pulse imaging of OH radicals in turbulent combustion because of its high pulse energy.     

Experimental analysis of local flame extinction in a turbulent jet diffusion flame by high repetition 2-D laser techniques and multi-scalar measurements

In this paper, we present a detailed experimental study of turbulence chemistry interactions in the “DLR_B” turbulent jet diffusion flame. The flame operates on mixtures of CH₄, H₂, and N₂ in the fuel stream at Re = 22,800 and is a target flame within the TNF workshop. Extinction and re-ignition events can be tracked in real time and related to the underlying flow field phenomena and temperature fields. Time resolved measurements of OH radical concentration fields are performed in combination with temperature and velocity field measurements. For this purpose, we combined high repetition rate (33 kHz) PLIF imaging with stereoscopic PIV and double pulse Rayleigh imaging techniques. Comparisons are made with results from multi-scalar Raman/Rayleigh/LIF point measurements that reveal the thermochemical state of the flame. The large deviations from equilibrium observed on resulting OH/temperature joint pdfs could be related to strain rate and Damköhler number variations caused by turbulent flow structures leading to frequent extinctions. The 2D measurement series uniquely reveal the underlying mechanism that can lead to such events. Finally, comparisons are made to strained laminar flame calculations, which are generally found to be in good agreement with the measured data.     

Lean or ultra-lean stretched planar methane/air flames

Lean premixed combustion has potential advantages of reducing pollutants and improving fuel economy. In some lean engine concepts, the fuel is directly injected into the combustion chamber resulting in a distribution of lean fuel/air mixtures. In this case, very lean mixtures can burn when supported by hot products from more strongly burning flames. This study examines the downstream interaction of opposed jets of a lean-limit CH₄/air mixture vs. a lean H₂/air flame. The CH₄ mixtures are near or below the lean flammability limit. The flame composition is measured by laser-induced Raman scattering and is compared to numerical simulations with detailed chemistry and molecular transport including the Soret effect. Several sub-limit lean CH₄/air flames supported by the products from the lean H₂/air flame are studied, and a small amount of CO₂ product (around 1% mole fraction) is formed in a “negative flame speed” flame where the weak CH₄/air mixture diffuses across the stagnation plane into the hot products from the H₂/air flame. Raman scattering measurements of temperature and species concentration are compared to detailed simulations using GRI-3.0, C₁, and C₂ chemical kinetic mechanisms, with good agreement obtained in the lean-limit or sub-limit flames. Stronger self-propagating CH₄/air mixtures result in a much higher concentration of product (around 6% CO₂ mole fraction), and the simulation results are sensitive to the specific chemical mechanism. These model-data comparisons for stronger CH₄/air flames improve when using either the C₂ or the Williams mechanisms.     

Laser Raman radar detection based on a sampling technique

A study is presented of the total differential Raman cross section for CO₂, O₂, CO, CH₄, H₂O and H₂ relative to that of N₂. The scattered radiation was collected perpendicularly to the excitation beam from a 337.1 nm nitrogen laser of 50 kW peak power. The short pulse with a duration of 2.5 ns was conveniently handled by a sampling oscilloscope. The sampling technique permits a smoothing process to be performed at the output of the sampling oscilloscope, which does not affect the time resolution, in order to improve the signal-to-noise ratio of the records of Raman spectra.     

Experimental and numerical investigation of microscale hydrogen diffusion flames

Characteristics of microscale hydrogen diffusion flames produced from sub-millimeter diameter (d = 0.2 and 0.48 mm) tubes are investigated using non-intrusive UV Raman scattering coupled with LIPF technique. Simultaneous, temporally and spatially resolved point measurements of temperature, major species concentrations (O₂, N₂, H₂O, and H₂), and absolute hydroxyl radical concentration (OH) are made in the microflames for the first time. The probe volume is 0.02 × 0.04 × 0.04 mm³. In addition, photographs and 2-D OH imaging techniques are employed to illustrate the flame shapes and reaction zones. Several important features are identified from the detailed measurements of microflames. Qualitative 2-D OH imaging indicates that a spherical flame is formed with a radius of about 1 mm as the tube diameter is reduced to 0.2 mm. Raman/LIPF measurements show that the coupled effect of ambient air leakage and pre-heating enhanced thermal diffusion of H₂ leads to lean-burn conditions for the flame. The calculated characteristic features and properties indicate that the buoyancy effect is minor while the flames are in the convection–diffusion controlled regime because of low Peclet number. Also, the effect of Peclet number on the flame shape is minor as the flame is in the convection–diffusion controlled regime. Comparisons between the predicted and measured data indicate that the trends of temperature, major species, and OH distributions are properly modeled. However, the code does not properly predict the air entrainment and pre-heating enhanced thermal-diffusive effects. Therefore, thermal diffusion for light species and different combustion models might need to be considered in the simulation of microflame structure.     

Reaction zone structures and mixing characteristics of partially premixed swirling CH4/air flames in a gas turbine model combustor

The mixing, reaction progress, and flame front structures of partially premixed flames have been investigated in a gas turbine model combustor using different laser techniques comprising laser Doppler velocimetry for the characterization of the flow field, Raman scattering for simultaneous multi-species and temperature measurements, and planar laser-induced fluorescence of CH for the visualization of the reaction zones. Swirling CH₄/air flames with Re numbers between 7500 and 60,000 have been studied to identify the influence of the turbulent flow field on the thermochemical state of the flames and the structures of the CH layers. Turbulence intensities and length scales, as well as the classification of these flames in regime diagrams of turbulent combustion, are addressed. The results indicate that the flames exhibit more characteristics of a diffusion flame (with connected flame zones) than of a uniformly premixed flame.     

Multi-kHz mixture fraction imaging in turbulent jets using planar Rayleigh scattering

In this study, we describe the development of two-dimensional, high repetition-rate (10-kHz) Rayleigh scattering imaging as applied to turbulent flows. In particular, we report what we believe to be the first sets of high-speed 2D Rayleigh scattering images in turbulent non-reacting jets, yielding temporally correlated image sequences of the instantaneous mixture fraction field. Results are presented for turbulent jets of propane issuing into a low-speed co-flow of air at jet-exit Reynolds numbers of 10,000, 15,000, and 30,000 at various axial positions downstream of the jet exit. The quantitative high-speed mixture fraction measurements are facilitated by the use of a calibrated, un-intensified, high-resolution CMOS camera in conjunction with a unique high-energy, high-repetition rate pulse-burst laser system (PBLS) at Ohio State, which yields output energies of ∼200 mJ/pulse at 532 nm with 100-μs laser pulse spacing. The quality, accuracy, and resolution of the imaging system and the resulting image sets are assessed by (1) comparing the mean mixture fraction results to known scaling laws for turbulent jets, (2) comparing instantaneous images/mixture fraction profiles acquired simultaneously with the high-speed CMOS camera and a well-characterized, high-quantum efficiency CCD camera, and (3) comparing statistical quantities such as the probability density function of the mixture fraction results using the high-speed CMOS camera and the CCD camera. Results indicate accurate mixture fraction measurements and a high potential for accurately measuring mixture fraction gradients in both time and space.     

Several applications of laser diagnostics for visualization of combustion phenomena

Several applications of laser diagnostic techniques to visualize combustion phenomena are presented, including reactive Mie scattering for flow, Rayleigh and Raman spectroscopy for major species, laser-induced fluorescence for minor species, and laser extinction, scattering, and laser-induced incandescence for soot. These techniques have been applied to diffusion flame oscillation, a recirculation zone in a burner, laminar and turbulent lifted flames, flame propagation along a vortex tube, and soot zone characteristics, to demonstrate the usefulness of the techniques to provide a better understanding of physical mechanisms.     

Phase-resolved laser Raman scattering and laser Doppler velocimetry applied to periodic instabilities in a gas turbine model combustor

The understanding of periodic flame instabilities belongs to the major challenges in modern combustion research and technology and is of special importance for lean premixed gas turbine combustion. This paper presents experimental investigations in a gas turbine model combustor using laser diagnostic techniques. A partially premixed CH₄/air flame operated at a thermal power of 10 kW at atmospheric pressure and an overall equivalence ratio of 0.75, which exhibited thermoacoustic oscillations at a frequency of 290 Hz, was investigated. Phase-locked laser Raman scattering was applied in order to determine the major species concentrations, temperature, and mixture fraction. In addition, laser Doppler velocimetry (LDV) was used separately for the measurement of the axial and radial velocity components. The measurements revealed pronounced phase-dependent variations of the velocity and the temperature, species, and mixture fraction distributions. The combined Raman and LDV results also enabled the determination of molecular species fluxes which showed that the fuel and air supply rates both varied during an oscillation cycle by ±33% but with a phase shift of 80 between them. The correlations between temperature and mixture fraction revealed strong deviations from equilibrium composition and temperature, and their phase-dependent changes reflected the transport and mixing processes near the nozzle. The emphasis of the paper lies on the demonstration of the potential of phase-locked laser Raman scattering for the study of phenomena of periodic flame instabilities. PACS 33.20; 39.30; 47.27; 47.70; 82.33; 82.40     

Single‐shot CARS thermometry of high‐pressure hydrocarbon flames using simultaneous intensity and linewidth measurements

We demonstrate the feasibility of single laser shot coherent anti‐Stokes Raman scattering thermometry with simultaneous measurement of intensities of hydrogen Q‐branch lines and their linewidths in a pulsed CH₄/O₂ combustion chamber operating at 20 MPa pressure and 3000 K temperature—parameters that are typical for full‐scale rocket engines. The measurements were done by means of a spectrograph combined with an interferometer having orthogonal directions of dispersions. This approach allows correct temperature evaluation that takes into account the directly measured linewidths. Copyright © 2010 John Wiley & Sons, Ltd.     

Homogeneous ignition of CH4/air and H2O and CO2-diluted CH4/O2 mixtures over Pt; an experimental and numerical investigation at pressures up to 16 bar

The homogeneous ignition of CH₄/air, CH₄/O₂/H₂O/N₂, and CH₄/O₂/CO₂/N₂ mixtures over platinum was investigated experimentally and numerically at pressures 4 bar p 16 bar, temperatures 1120 K T 1420 K, and fuel-to-oxygen equivalence ratios 0.30 0.40. Experiments have been performed in an optically accessible catalytic channel-flow reactor and included planar laser induced fluorescence (LIF) of the OH radical for the determination of homogeneous (gas-phase) ignition and one-dimensional Raman measurements of major species concentrations across the reactor boundary layer for the assessment of the heterogeneous (catalytic) processes preceding homogeneous ignition. Numerical predictions were carried out with a 2D elliptic CFD code that included elementary heterogeneous and homogeneous chemical reaction schemes and detailed transport. The employed heterogeneous reaction scheme accurately captured the catalytic methane conversion upstream of the gaseous combustion zone. Two well-known gas-phase reaction mechanisms were tested for their capacity to reproduce measured homogeneous ignition characteristics. There were substantial differences in the performance of the two schemes, which were ascribed to their ability to correctly capture the p–T– parameter range of the self-inhibited ignition behavior of methane. Comparisons between measured and predicted homogeneous ignition distances have led to the validation of a gaseous reaction scheme at 6 bar p 16 bar, a pressure range of particular interest to gas-turbine catalytically stabilized combustion (CST) applications. The presence of heterogeneously produced water chemically promoted the onset of homogeneous ignition. Experiments and predictions with CH₄/O₂/H₂O/N₂ mixtures containing 57% per volume H₂O have shown that the validated gaseous scheme was able to capture the chemical impact of water in the induction zone. Experiments with CO₂ addition (30% per volume) were in good agreement with the numerical simulations and have indicated that CO₂ had only a minor chemical impact on homogeneous ignition.     

Simultaneous measurement of localized heat release with OH/CH2O-LIF imaging and spatially integrated OH∗ chemiluminescence in turbulent swirl flames

The in-situ and localized observation of heat release in turbulent flames is important for the validation of computational modeling of turbulent flows with combustion. In the present work we obtain localized information on heat release rate (HRR) by the commonly accepted technique of the simultaneous and single-shot planar imaging of OH and CH₂O concentrations by laser-induced fluorescence (LIF). Additionally, we combine this with the simultaneous line-of-sight and temporally resolved chemiluminescence detection of OH^?, spatially integrated within the flame volume, interrogated by the laser sheets used for the HRR imaging technique. The combined diagnostic methods are demonstrated for a swirl-stabilized, premixed turbulent methane/air flame of 30-kW thermal power, and they show the existence of correlations between both HRR-sensitive diagnostic techniques.     

三角激光脉冲尾波加速粒子模拟

电子俘获是激光尾波场加速电子的主要机理，增大电子的初速度可以使更多的电子被尾波场俘获.提出三角脉冲激发尾波加速电子的方案，三角脉冲平缓上升沿激发受激Raman散射，用以初步加速电子，三角脉冲陡峭下降沿激发尾波场，将更多的电子加速到接近光速.2D3V粒子模拟结果证实了这一点.同时表明：脉冲长度为几个等离子体波长的超强激光在稀薄等离子体中传播时，还激发侧向Raman散射.在侧向受激Raman散射中，静电波增长最快的波矢模式为k_p=(2ω_p/ω₀ 关键词： 有质动力 电子俘获 前向受激Raman散射 侧向受激Raman散射     

Flame structure of laminar premixed anisole flames investigated by photoionization mass spectrometry and photoelectron spectroscopy

Two laminar, premixed, fuel-rich flames fueled by anisole-oxygen-argon mixtures with the same cold gas velocity and pressure were investigated by molecular-beam mass spectrometry at two synchrotron sources where tunable vacuum-ultraviolet radiation enables isomer-resolved photoionization. Decomposition of the very weak O–CH₃ bond in anisole (C₆H₅OCH₃) by unimolecular decomposition yields the resonantly-stabilized phenoxy radical (C₆H₅O). This key intermediate species opens reaction routes to five-membered ring species, such as cyclopentadiene (C₅H₆) and cyclopentadienyl radicals (C₅H₅). Anisole is often discussed as model compound for lignin to study the phenolic-carbon structure in this natural polymer. Measured temperature profiles and mole fractions of many combustion intermediates give detailed information on the flame structure. A very comprehensive reaction mechanism from the literature which includes a sub-scheme for anisole combustion is used for species modeling. Species with the highest measured mole fractions (on the order of 10^?3–10^?2) are CH₃, CH₄, C₂H₂, C₂H₄, C₂H₆, CH₂O, C₅H₅ (cyclopentadienyl radical), C₅H₆ (cyclopentadiene), C₆H₆ (benzene), C₆H₅OH (phenol), and C₆H₅CHO (benzaldehyde). Some are formed in the first destruction steps of anisole, e.g., phenol and benzaldehyde, and their formation will be discussed and with regard to the modeling results. There are three major routes for the fuel destruction: (1) formation of benzaldehyde (C₆H₅CHO), (2) formation of phenol (C₆H₅OH), and (3) unimolecular decomposition of anisole to phenoxy (C₆H₅O) and CH₃ radicals. In the experiment, the phenoxy radical could be measured directly. The phenoxy radical decomposes via a bicyclic structure into the soot precursor C₅H₅ and CO. Formation of larger oxygenated species was observed in both flames. One of them is guaiacol (2-methoxyphenol), which decomposes into fulvenone. The presented speciation data, which contain more than 60 species mole fraction profiles of each flame, give insights into the combustion kinetics of anisole.     

New far-infrared laser lines from CH3Cl and CH3Br optically pumped with a continuously tunable high pressure CO2 laser

In this paper we report on the detection of new far-infrared laser lines from CH₃Cl and CH₃Br optically pumped with a continuously tunable high pressure CO₂ laser. We found 80 new lines for CH₃Cl and 9 new lines for CH₃Br in the frequency region between 16 cm^–1 and 41 cm^–1, all due to stimulated Raman scattering. For the Raman gain regions bandwidths up to about 700 MHz were found. We also observed high intensity short far-infrared laser pulses of durations in the nanosecond regime.Permanent address: Physics Department, State Pedagogical University, SU-119435 Moscow, USSR