CARS investigation of collisional shift of the hydrogen Q‐branch transitions by water at high temperatures

A high‐resolution (∼0.1 cm⁻¹) spectroscopic method based on the application of a Fabry–Pérot interferometer to the spectral analysis of the coherent anti‐Stokes Raman scattering (CARS) signal from an individual Raman transition was used to obtain single‐shot spectra of hydrogen Q‐branch transitions directly in the flame of a pulsed, high‐pressure H₂/O₂ combustion chamber. Simultaneously with the Fabry–Pérot pattern, a broadband CARS spectrum of the complete H₂Q ‐branch structure was recorded in order to measure the temperature of the probe volume. During every cycle of the combustion chamber, a pressure pulse together with single‐shot CARS spectra, providing information on individual line shapes and medium temperature, was recorded. On the basis of the experimental data, the temperature dependences of lineshift coefficients for several Q‐branch lines of hydrogen molecules under collisions with water molecules were determined in the temperature range 2100 < T < 3500 K, and an empirical ‘fitting law’ for H₂ H₂O lineshift coefficients is proposed. Copyright © 2010 John Wiley & Sons, Ltd.     

Investigation on spherically expanding flame temperature of n-butane/air mixtures with tunable diode laser absorption spectroscopy

A joint schlieren imaging, pressure recording and tunable diode laser absorption spectroscopy (TDLAS) thermometry technique was developed to simultaneously determine the flame radius, pressure and line-of-sight averaged temperature of spherically expanding flames of n-butane/air mixtures at initial temperature of 298 K, initial pressure of 1 atm and equivalence ratios of 0.9–1.5. To probe the flame temperature, a mid-infrared interband cascade laser at 4.2 µm was used to measure the time-resolved direct absorption spectra of CO₂ which are strongly related to flame temperature, CO₂ mole fraction, flame radius and pressure. Quantitative line-of-sight averaged temperatures of burnt gas were obtained by fitting the normalized absorbance spectra. Three typical stages, including the spark affected initial stage, quasi-steady stage and the pressure induced growing stage are determined from the evolution of measured temperature as a function of time and flame radius. The relation between flame temperature, stretch rate and burning velocity of burnt gas are analyzed. Stretch rate is found to have minor effect on the measured temperature in the quasi-steady stage. The relative variation of temperature is much smaller than that of velocity. The flame with lower normalized temperature tends to propagate slower.     

The application of single-pulse CARS for temperature measurements in a turbulent stagnation flame

N₂ Q-branch CARS spectra have been recorded and evaluated for temperature determination in a turbulent, premixed CH₄/air stagnation flame with a burner of 40 mm diameter and 22 kW thermal load. Temperature histograms on the flame axis at different distances from the stagnation plate have been measured. Problems of practical applicability are addressed, including those arising from the limited spatial resolution of the BOXCARS geometry, from an insufficient dynamic range of the diode array detector, and from a memory effect of the detector in the case of measurements in highly turbulent flame areas with strong intermittency. Some information is given on the computerized acquisition and on the evaluation of the large amounts of data that are necessary for extensive investigations in large combustion systems.     

UV raman spectroscopy of H2-air flames excited with a narrowband KrF laser

Raman spectra of H₂ and H₂O in flames excited by a narrowband KrF excimer laser are reported. Observations are made over a porous-plug, flat-flame burner reacting H₂ in air, fuel-rich with nitrogen dilution to control the temperature, and with a H₂ diffusion flame. Measurements made from UV Raman spectra show good agreement with measurements made by other means, both for gas temperature and relative major species concentrations. Laser-induced fluorescence interferences arising from OH and O₂ are observed in emission near the Raman spectra. These interferences do not preclude Raman measurements, however.     

Numerical study on flame spread of an n-decane droplet array in different temperature environment under microgravity

A series of numerical calculations of flame spread of an n-decane droplet array was conducted at different ambient temperatures (T_a = 300 and 573 K) for S/d₀ from 1.5 to 10, where S is the droplet interval and d₀ is the initial droplet diameter. The authors compared these numerical results with experimental results under similar conditions at different ambient temperatures for the first time in this study. Good qualitative agreement in flame spread behavior between numerical results and microgravity experiments is obtained. Flame spread mode changed with an increase in S/d₀. Also, appearance of the flame spread mode in a stepping-stone manner (Mode III in [Jpn. Soc. Mech. Eng. 68 (672) (2002) 2423]) in a normal temperature environment was verified by numerical calculations and microgravity experiments, although it was not predicted in the theoretical analysis. In addition, good qualitative agreement of flame spread rate V_f versus S/d₀ was obtained between numerical and experimental results, although numerical results were at least twice as large as experimental results. V_f had a maximum peak at a specific S/d₀ for a different ambient temperature. Employment of improved reaction model and consideration for thermal radiation heat transfer are expected to produce quantitatively better results. An increase in surface temperature of unburned droplets and the development of a flammable gas layer around the droplets were promoted in a high-temperature environment, due to an increase in heat transfer from ambient air to the droplet. As a result, V_f was increased by the higher ambient temperature, suggesting that ambient temperature plays a significant role both in the flame spread mode and the flame spread rate through promotion of a flammable gas layer around unburned droplets.     

Laser-induced fluorescence determination of flame temperatures in comparison with CARS measurements

Temperature profiles in several premixed low pressure H₂/O₂/N₂ flames and in an atmospheric pressure CH₄/air flame were determined by laser-induced fluorescence (LIF) and by CARS experiments. In the LIF study, temperatures were derived from OH excitation spectra, CARS temperatures were deduced from N₂ Q-branch spectra. The present study is the first quantitative comparison of these two methods for temperature determination in flames burning at pressures up to 1 bar. The resulting temperatures showed good agreement.     

Rotational CARS for simultaneous measurements of temperature and concentrations of N2, O2, CO, and CO2 demonstrated in a CO/air diffusion flame

Rotational coherent anti-Stokes Raman spectroscopy (CARS) has over the years demonstrated its strong potential to measure temperature and relative concentrations of major species in combustion. A recent work is the development and experimental validation of a CO₂ model for thermometry, in addition to our previous rotational CARS models for other molecules. In the present work, additional calibration measurements for relative CO₂/N₂ concentrations have been made in the temperature range 294-1246 K in standardized CO₂/N₂ mixtures. Following these calibration measurements, rotational CARS measurements were performed in a laminar CO/air diffusion flame stabilized on a Wolfhard-Parker burner. High-quality spectra were recorded from the fuel-rich region to the surrounding hot air in a lateral cross section of the flame. The spectra were evaluated to obtain simultaneous profiles of temperature and concentrations of all major species; N₂, O₂, CO, and CO₂. The potential for rotational CARS as a multi-species detection technique is discussed in relation to corresponding strategies for vibrational CARS.     

Absolute radical concentration measurements in low-pressure H2/O2 flames during the combustion of graphite

Absolute CN and CH radical concentrations were determined in situ during the combustion of a graphite substrate in premixed, laminar, low-pressure, H₂/O₂ flames for two different equivalence ratios, = 1.0 and = 1.5. For CN measurements, a small amount of NO (1.8%) was added. The concentration of CN was measured by cavity ring-down spectroscopy (CRDS) probing the absorption of the P_1,2 (13) in the B–X (0, 0) band at 388.1 nm, and the concentration of CH was measured by linear unsaturated laser-induced fluorescence (LIF) exciting the fluorescence of the R₁ (4) in the B–X (0, 0) band at 387.4 nm. Temperature measurements were done based on LIF excitation spectra of OH in the A–X (0, 0) band. It was found that the graphite substrate reduces the flame temperature in the vicinity of its surface. The CN concentrations were found to be three times higher for the rich flame than for the stoichiometric flame. CH concentrations were slightly higher for the stoichiometric flame than for the rich flame. The observed CH/CN concentration ratio is substantially lower compared to NO-doped low-pressure CH₄/O₂ flames. The obtained quantitative information can serve as a first calibration point for detailed numerical simulations of the burning solid graphite, which are based on the concept of surface elementary reactions.     

On the stability of one-dimensional diffusion flames established between plane,parallel, porous walls

A one-dimensional, non-premixed flame stability analysis is undertaken.Oscillatory and cellular flame instabilities are identified by a careful studyof the numerically calculated eigenvalues of the linearized system of equations. The numerical investigation details the critical locations for changes in flame behaviour, as well as the critical values of variousparameters that affect flame stability. A critical Lewis number, greaterthan unity, is identified as the value where unstable oscillations maybegin to appear (Le?>?Le _c) and for which cellular flames can exist(Le?<?Le _c). Some prior discussions are clarified regarding theaforementioned critical values, as well as the role of convection inproducing flame instabilities. The methodology of the stability analysis isdiscussed in detail.     

Raman spectroscopic study of a laminar hydrogen diffusion flame in air

Spontaneous Raman spectroscopy has been employed for time-averaged, spatially-resolved measurements of temperature and species concentration in an axisymmetric, laminar hydrogen diffusion flame in quiescent air. Temperatures were obtained from vibrational Q-branch raman spectra of N₂, O₂, and H₂ and the rotational Raman spectra of N₂ and H₂, and concentrations of H₂, and N₂ were determined. The results are compared to existing numerical nonequilibrium calculations for the conditions of this experiment. Significant differences between experimental and predicted temperature and concentration profiles are observed. In particular, the flame is larger in both diameter and length and the flame zone is thicker than predicted. Some possible sources of the discrepancies are discussed.     

Numerical investigation of flame–vortex interactions in laminar cross-flow non-premixed flames in the presence of bluff bodies

Flame stabilisation in a combustor having vortices generated by flame holding devices constitutes an interesting fundamental problem. The presence of vortices in many practical combustors ranging from industrial burners to high speed propulsion systems induces vortex–flame interactions and complex stabilisation conditions. The scenario becomes more complex if the flame sustains after separating itself from the flame holder. In a recent study [P.K. Shijin, S.S. Sundaram, V. Raghavan, and V. Babu, Numerical investigation of laminar cross-flow non-premixed flames in the presence of a bluff-body, Combust. Theory Model. 18, 2014, pp. 692–710], the authors reported details of the regimes of flame stabilisation of non-premixed laminar flames established in a cross-flow combustor in the presence of a square cylinder. In that, the separated flame has been shown to be three dimensional and highly unsteady. Such separated flames are investigated further in the present study. Flame–vortex interactions in separated methane–air cross flow flames established behind three bluff bodies, namely a square cylinder, an isosceles triangular cylinder and a half V-gutter, have been analysed in detail. The mixing process in the reactive flow has been explained using streamlines of species velocities of CH₄ and O₂. The time histories of z-vorticity, net heat release rate and temperature are analysed to reveal the close relationship between z-vorticity and net heat release rate spectra. Two distinct fluctuating layers are visible in the proper orthogonal decomposition and discrete Fourier transform of OH mass fraction data. The upper fluctuating layer observed in the OH field correlates well with that of temperature. A detailed investigation of the characteristics of OH transport has also been carried out to show the interactions between factors affecting fluid dynamics and chemical kinetics that cause multiple fluctuating layers in the OH.     

Stabilization mechanism of turbulent premixed flames in strongly swirled flows

The stabilization of turbulent premixed flames in strongly swirled flows undergoing vortex breakdown is studied in the case of the ALSTOM En-Vironmental (EV) double cone burner using a simple one-dimensional boundary layer type model and computational fluid dynamics, mainly at the level of large-eddy simulation. The analysis shows that, due to flame curvature effects, the flame speed on the combustor axis is 2 D _t/R _F lower than the turbulent burning rate, where D _t is a characteristic turbulent diffusion coefficient and R _F the flame radius of curvature. Flame propagation with negative speed observed in the experiments, i.e. the flame completely embedded in the central recirculation zone on the symmetry axis, is explained with the one-dimensional model as caused by the factor 2 D _t/R _F being larger than the characteristic turbulent burning rate. A peculiar sudden displacement of the flame anchoring location deep into the burner, which takes place experimentally at a critical value of the equivalence ratio, cannot however be explained with the present one-dimensional approach due to the modelling assumptions. The mathematical analysis is supported in this case with large-eddy simulation which can accurately reproduce the flame behaviour across the full operating range. It is finally shown that steady RANS methods cannot cope with the problem due to their inability to correctly predict the velocity flowfield in this burner.     

High-repetition rate measurements of temperature and thermal dissipation in a non-premixed turbulent jet flame

High-repetition rate laser Rayleigh scattering is used to study the temperature fluctuations, power spectra, gradients, and thermal dissipation rate characteristics of a non-premixed turbulent jet flame at a Reynolds number of 15,200. The radial temperature gradient is measured by a two-point technique, whereas the axial gradient is measured from the temperature time-series combined with Taylor’s hypothesis. The temperature power spectra along the jet centerline exhibit only a small inertial subrange, probably because of the low local Reynolds number (Re_δ ≈ 2000), although a larger inertial subrange is present in the spectra at off-centerline locations. Scaling the frequency by the estimated Batchelor frequency improves the collapse of the dissipation region of the spectra, but this collapse is not as good as is obtained in non-reacting jets. Probability density functions of the thermal dissipation are shown to deviate from lognormal in the low-dissipation portion of the distribution when only one component of the gradient is used. In contrast, nearly log-normal distributions are obtained along the centerline when both axial and radial components are included, even for locations where the axial gradient is not resolved. The thermal dissipation PDFs measured off the centerline deviate from log-normal owing to large-scale intermittency. At one-half the visible flame length, the radial profile of the mean thermal dissipation exhibits a peak off the centerline, whereas farther downstream the peak dissipation occurs on the centerline. The mean thermal dissipation on centerline is observed to increase linearly with downstream distance, reach a peak at the location of maximum mean centerline temperature, and then decrease for farther downstream locations. Many of these observed trends are not consistent with equivalent non-reacting turbulent jet measurements, and thus indicate the importance of understanding how heat release modifies the turbulence structure of jet flames.     

Two-dimensional imaging of glyoxal (C2H2O2) in acetylene flames using laser-induced fluorescence

2 H₂O₂). Laser-induced fluorescence spectra from glyoxal vapor using the same excitation wavelength of 428 nm showed the same strongest lines as the signal from the flame. Glyoxal was visualized in two different modes; two-dimensional imaging and a spatial-spectral mode where spectra were obtained at different spatial positions in the flame simultaneously. For the premixed laminar rich flame it is shown that glyoxal is produced early in the flame, before the signals for C₂ and CH appear. For the turbulent non-premixed flames it is shown that glyoxal is produced in a layer on the fuel rich side of the flames. Here the fuel is premixed with ambient air. This layer is thin and has a high spatial resolution. The general trend was that the glyoxal signal appeared in regions with a lower temperature compared with the emission from C₂ and CH. The imaging of glyoxal in turbulent acetylene flames is a promising tool for achieving new insight into flame phenomena, as it gives very good structural information on the flame front. Tests so far do not indicate that the detected glyoxal is a result of photo-production. To our knowledge, this is the first detection of glyoxal in flames using laser-induced fluorescence. Received: 19 December 1996/Revised version: 26 May 1997     

Thermal dileptons from quark and hadron phases of an expanding fireball

A fireball model with time evolution based on transport calculations is used to examine the dilepton emission rate of an ultra-relativistic heavy-ion collision. A transition from hadronic matter to a quark-gluon plasma at a critical temperature T _C between 130-170 MeV is assumed. We also consider a possible mixed phase scenario. We include thermal corrections to the hadronic spectra below T _C and use perturbation theory above T _C. The sensitivity of the spectra with respect to the freeze-out temperature, the initial fireball temperature and the critical temperature is investigated. Received: 4 August 2000 / Accepted: 14 November 2000     

In situ Raman characterization of nanoparticle aerosols during flame synthesis

Raman spectroscopy is applied to diagnose nanoparticle presence and characteristics in a gaseous flow field. Specifically, in situ monitoring of the Raman-active modes of TiO₂ and Al₂O₃ nanoparticles in aerosol form is demonstrated in high-temperature flame environments. This technique serves as a sensitive and reliable way to characterize particle composition and crystallinity (e.g. anatase versus rutile) and delineate the phase conversion of nanoparticles as they evolve in the flow field. The effect of temperature on the solid-particle Raman spectra is investigated by seeding nanoparticles into a co-flow jet diffusion flame, where local gas-phase temperatures are correlated by shape-fitting the N₂ vibrational Stokes Q-branch Raman spectra. Applying the technique to a flame synthesis environment, the results demonstrate that in situ Raman of as-formed nanoparticles can be readily applied to other gas-phase synthesis systems, especially as an on-line diagnostic.     

CO2 addition and pressure effects on laminar and turbulent lean premixed CH4 air flames

An experimental study on CH₄–CO₂–air flames at various pressures is conducted by using both laminar and turbulent Bunsen flame configurations. The aim of this research is to contribute to the characterization of fuel lean methane/carbon dioxide/air premixed laminar and turbulent flames at different pressures, by studying laminar and turbulent flame propagation velocities, the flame surface density and the instantaneous flame front wrinkling parameters. PREMIX computations and experimental results indicate a decrease of the laminar flame propagation velocities with increasing CO₂ dilution rate. Instantaneous flame images are obtained by Mie scattering tomography. The image analysis shows that although the height of the turbulent flame increases with the CO₂ addition rate, the flame structure is quite similar. This implies that the flame wrinkling parameters and flame surface density are indifferent to the CO₂ addition. However, the pressure increase has a drastic effect on both parameters. This is also confirmed by a fractal analysis of instantaneous images. It is also observed that the combustion intensity S_T/S_L increases both with pressure and the CO₂ rate. Finally, the mean fuel consumption rate decreases with the CO₂ addition rate but increases with the pressure.     

Effect of local variations of the laminar flame speed on the global finger-flame acceleration scenario

Numerous formulations describing the dynamics and morphology of corrugated flames, including the scenarios of flame acceleration, are based on a “geometrical consideration”, where the wrinkled-to-planar flame velocities ratio, S_w /S_L , is evaluated as the scaled flame surface area, while the entire combustion chemistry is immersed into the planar flame speed S_L , which is assumed to be constant. However, S_L may experience noticeable spatial/temporal variations in practice, in particular, due to pressure/temperature variations as well as non-uniform distribution of the equivalence ratio and/or that of combustible or inert dust impurities. The present work initiates the systematic study of the impact of the local S_L -variations on the global flame evolution scenario. The variations are assumed to be imposed externally, in a manner being a free functional of the formulation. Specifically, the linear, parabolic and hyperbolic spatial S_L -distributions are incorporated into the formulations of finger flame acceleration in pipes, and they are compared to the case of constant S_L . Both two-dimensional channels and cylindrical tubes are considered. The conditions promoting or moderating flame acceleration are identified, and the revisited equations for the flame shape, velocity and acceleration rate are obtained for various S_L -distributions. The theoretical findings are validated by the computational simulations of the reacting flow equations, with agreement between the theory and modelling demonstrated.     

Unsteady deflagration speed of an auto-ignitive dimethyl-ether (DME)/air mixture at stratified conditions

The propagation speed of an auto-ignitive dimethyl-ether (DME)/air mixture at elevated pressures and subjected to monochromatic temperature oscillations is numerically evaluated in a one-dimensional statistically stationary configuration using fully resolved numerical simulations with reduced kinetics and transport. Two sets of conditions with temperatures within and slightly above the negative temperature coefficient (NTC) regime are simulated to investigate the fundamental aspects of auto-ignition and flame propagation along with the transition from auto-ignitive deflagration to spontaneous propagation regimes under thermal stratification. Contrary to the standard laminar flame speed, the steady propagation speed of an auto-ignitive front is observed to scale proportionally to its level of upstream reactivity. It is shown that this interdependence is primarily influenced by the characteristic residence time and the homogeneous auto-ignition delay. Furthermore, the unsteady reaction front in either of the two cases responds distinctly to the imposed stratification. Specifically, the results in both cases show that the dynamic flame response depends on the mean temperature at the flame base T_b and the time-scale of thermal stratification. It is also found that, based on T_b and the propensity of the mixture to two-stage chemistry, the instantaneous peak propagation speed and the overall time taken to achieve that speed differs considerably. A displacement speed analysis is carried out to elucidate the underlying combustion modes that are responsible for such a variation in flame response.     

Flame front analysis of high-pressure turbulent lean premixed methane–air flames

An experimental study on lean turbulent premixed methane–air flames at high pressure is conducted by using a turbulent Bunsen flame configuration. A single equivalence ratio flame at Φ = 0.6 is explored for pressures ranging from atmospheric pressure to 0.9 MPa. LDA measurements of the cold flow indicate that turbulence intensities and the integral length scale are not sensitive to pressure. Due to the decreased kinematic viscosity with increasing pressure, the turbulent Reynolds numbers increase, and isotropic turbulence scaling relations indicate a large decrease of the smallest turbulence scales. Available experimental results and PREMIX code computations indicate a decrease in laminar flame propagation velocities with increasing pressure, essentially between the atmospheric pressure and 0.5 MPa. The u′/S_L ratio increases therefore accordingly. Instantaneous flame images are obtained by Mie scattering tomography. The images and their analysis show that pressure increase generates small scale flame structures. In an attempt to generalize these results, the variance of the flamelet curvatures, the standard deviation of the flamelet orientation angle, and the flamelet crossing lengths have been plotted against which is proportional to the ratio between the integral and Taylor length scales, and which increases with pressure. These three parameters vary linearly with the ratio between large and small turbulence scales and clearly indicate the strong effect of this parameter on premixed turbulent flame dynamics and structure. An obvious consequence is the increase in flame surface density and hence burning rate with pressure, as confirmed by its direct determination from 2D tomographic images.