Time-resolved LIF of OH in the flame front of premixed and diffusion flames at atmospheric pressure

Time-resolved fluorescence measurements are reported for the OH radical in the flame fronts of laminar atmospheric pressure flames. Effective (collision-limited) lifetimes were determined following excitation of theA ²⁺, = 0 state of OH using a picosecond dye-laser system based on the distributed-feedback principle. Measurements were made in a premixed knife-edge burner for rich CH₄/N₂O/N₂ and CH₄/air flames and in a counterflow diffusion burner for a CH₄/air flame. In the accessible range, results indicate a net dependence of lifetime on temperature intermediate betweenT andT ^0.5 for these flames.     

Quantitative one-dimensional single-pulse multi-species concentration and temperature measurement in the lift-off region of a turbulent H2/air diffusion flame

In this article, we report on one-dimensional single-pulse measurements of temperature and major-species concentration (O₂, N₂, H₂O and H₂) in a turbulent H₂/air jet diffusion flame using Raman and Rayleigh scattering of KrF* excimer-laser radiation. Spatial resolution of 0.5 mm along a 6mm long line has been obtained, with reasonable error limits for mole fraction ( = 5 % for N₂ detection) and temperature (T = 8 %) determination at flame temperatures. We present various profiles showing the composition and temperature along a line at different heights in the flame with particular emphasis on the lift-off region (i.e. lowx/D). In this zone, temperature and mixture fraction can be determined simultaneously — from a single laser pulse — in a spatial region extending from unburnt gas in the center of the jet across the flame front into the cool air of the surrounding atmosphere. This allows for the first time the systematic study of the shape and width of the high-temperature region and the corresponding concentration and temperature gradients. The comparison of averaged data and scatter plots with previous pointwise measurements shows good agreement.     

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.     

The role of methylene in prompt NO formation

We address the plausibility of singlet methylene (¹CH₂) in the prompt NO formation mechanism via examination of experimental species profiles and kinetic flame modeling of several low-pressure methane-oxygen-nitrogen flames. Existing kinetic models assuming CH as the only prompt NO precursor greatly underpredict NO formation under very fuel-lean conditions. We have constructed a kinetic pathway initiated by the recombination of singlet CH₂ with molecular nitrogen to form diazomethane, CH₂NN, early in the flame. Although the majority of the diazomethane is predicted to react with flame radicals to regenerate N₂, a small percentage (approximately 10%) is predicted to react via cleavage of the NN bond leading to NO formation. This leads to accurate prediction of the experimental measurements of NO formation in lean, low-pressure flames. Assuming reasonable kinetic parameters for the reactions of CH₂, the large underprediction of NO under lean conditions can be rectified by the inclusion of the ¹CH₂ prompt NO pathway in the kinetic mechanism.     

Far-infrared laser stark spectroscopy of CH3OH and13CH3OH

The high resolution laser Stark spectra of methanol and¹³C-substituted methanol have been studied up to Stark fields of about 60 000V/cm with the HCN and DCN lasers. Numerous families of absorption lines have been observed in both parallel and perpendicular polarizations. For methanol, the transitions J _k =7₅ 6₄ A, _t=0; J _k =11₄ 10₃ E _l , _t=0; and J _k =17₃ 16₂ E₂, _t=0 have been identified while the assignments for¹³C-substituted methanol are J _k =14₈ 15₇ A, _t=0; J _k =15₃ 14₂ A⁺, _t=0; J _k =10₇ 9₆ A, _t=0; and J _k =27₉ 27₈ E₁, _t=0. Zero-field frequencies for the assigned transitions are given with improved accuracy over those calculated from available molecular constants, especially for¹³CH₃OH.     

Observation of new laser transitions and saturation effects in optically pumped NO

We report investigations of an NO laser employing specially profiled magnetic fields of up to 3.4T, and F₂ pump laser intensities as great as 20 MW cm^–2. We have observed laser oscillation at 226 nm on a rotational branch of the B'-X/it(3–11) band of NO for the first time, in addition to the previously reported oscillation at 218 nm on the B'-X/it(3–10) band. We have also observed visible laser emission on a rotational branch of the B ²-B ² II(3–1) band of NO. Saturation of the NO laser pulse energy with pump intensity has been observed, the total NO laser pulse energy having been increased to 490 J. The possibility of increasing the NO laser pulse energy towards 1 mJ per transition is discussed.     

Critical temperature and reactant mass flux for radiative extinction of ethylene microgravity spherical diffusion flames at 1 bar

In microgravity combustion, where buoyancy is not present to accelerate the flow field and strain the flame, radiative extinction is of fundamental importance, and has implications for spacecraft fire safety. In this work, the critical point for radiative extinction is identified for normal and inverse ethylene spherical diffusion flames via atmospheric pressure experiments conducted aboard the International Space Station, as well as with a transient numerical model. The fuel is ethylene with nitrogen diluent, and the oxidizer is an oxygen/nitrogen mixture. The burner is a porous stainless-steel sphere. All experiments are conducted at constant reactant flow rate. For normal flames, the ambient oxygen mole fraction was varied from 0.2 to 0.38, burner supply fuel mole fraction from 0.13 to 1, total mass flow rate, ṁ_total, from 0.6 to 12.2 mg/s, and adiabatic flame temperature, T_ad, from 2000 to 2800 K. For inverse flames, the ambient fuel mole fraction was varied from 0.08 to 0.12, burner supply oxygen mole fraction from 0.4 to 0.85, ṁ_total from 2.3 to 11.3 mg/s, and T_ad from 2080 to 2590 K. Despite this broad range of conditions, all flames extinguish at a critical extinction temperature of 1130 K, and a fuel-based mass flux of 0.2 g/m²-s for normal flames, and an oxygen-based mass flux of 0.68 g/m²-s for inverse flames. With this information, a simple equation is developed to estimate the flame size (i.e., location of peak temperature) at extinction for any atmospheric-pressure ethylene spherical diffusion flame given only the reactant mass flow rate. Flame growth, which ultimately leads to radiative extinction if the critical extinction point is reached, is attributed to the natural development of the diffusion-limited system as it approaches steady state and the reduction in the transport properties as the flame temperature drops due to increasing flame radiation with time (radiation-induced growth.)     

Prediction of NO in turbulent diffusion flames using Eulerian particle flamelet model

The combustion characteristics for the turbulent diffusion flames using the unsteady flamelet concept have been numerically investigated. The Favre-averaged Navier–Stokes equations are solved by a finite volume method of SIMPLE type that incorporates the laminar flamelet concept with a modified k ? ε turbulence model. The NO formation is estimated by solving the Eulerian particle transport equations in a postprocessing mode. Two test problems are considered: CH₄/H₂/N₂ jet flame and CH₄/H₂ stabilised bluff body flame. The temperature and species profiles are well captured by the flamelet model. Two different chemical mechanisms (GRI 2.11 and 3.0) give nearly identical results for temperature and species except NO. The GRI 3.0 gives significantly higher NO levels compared to the GRI 2.11. This is mainly attributed to the difference in NO formation by the prompt mechanism. The NO formation is sensitive to the number of flamelet particles. The NO levels for two test flames do not change when the flamelet particle number exceeds six.     

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.     

Linewidth studies on the Kr+ 469.4 nm and 473.9 nm lines excited in a helium-krypton hollow cathode discharge

Collisional and Doppler linewidths (v _C and v _D ) of the 469.4 nm and 473.9 nm Kr ion lines were measured in a He-Kr hollow cathode discharge using Fabry-Perot technique. A linear dependence of v _C on He pressure was found for both lines. Significant differences were found between the temperature values deduced from the v _D -s of the two lines, and an unexpected temperature dependence of the broadening parameter for the Kr⁺ 469 nm line was also observed. The temperature difference between the two lines is explained by excitation of the upper level of the 469 nm line by second kind collisions between metastable He atoms and ground-state Kr ions, while the temperature dependence of the broadening parameter of the Kr⁺ 469 nm line is suggested to be due to the inverse process.     

Flame stabilization in high pressure LOx/GH2 and GCH4 combustion

Planar laser induced fluorescence (PLIF) of OH is used to examine flame stabilization in high pressure cryogenic flames formed by injecting a central jet of low speed liquid oxygen surrounded by a high speed gaseous stream of hydrogen or methane. In the LO_x/GH₂ experiments injection conditions are transcritical as the chamber pressure is above critical but the temperature is below critical . In the LO_x/GCH₄ experiments the chamber pressure and LO_x injection temperature are below critical , . Hydrogen or methane are injected at room temperature LIF images delineate the flame edge in the injector nearfield. The two flames are stabilized in the vicinity of the liquid oxygen injector lip but the anchor point is found to lie closer to the lip in the LO_x/GH₂ case and its displacement from shot to shot is of a smaller amplitude than that corresponding to the LO_x/GCH₄ flame. Interpretation of these data is based on a previous analysis which indicates that stabilization is essentially controlled by a dimensionless group formed by comparing the lip thickness to the flame edge thickness Ψ = h_s/δ_f. It is found that Ψ slightly exceeds unity in the LO_x/GH₂ case essentially fulfilling the stability condition while Ψ < 1 in the LO_x/GCH₄ case. In this last situation the flame is thicker than the characteristic thickness h_s and it is therefore sensitive to the high speed methane stream. Anchoring is imperfect and the flame edge moves with the turbulent eddies shed from the lip. Global stabilization is achieved dynamically but the reactive layer is not well established and the large amplitude motion of the edge is a symptom of a possible lift-off. Theoretical estimates indicate that LO_x/GCH₄ flame stabilization requires a thicker lip size than the LO_x/GH₂ propellant couple.     

Phase-matched third-harmonic generation of Nd: Glass-laser picosecond pulses in a new cyanine-dye solution

The phase-matched direct tripling of picosecond light pulses of a mode-locked Nd: glass laser in a new cyanine dye PMC is studied. The solvents trifluoroethanol (TFE) and hexafluoroisopropanol (HFIP) are applied. The S ₀–S ₁ absorption peak of the dye is around =480 nm and the absorption cross section at the third-harmonic wavelength of ₃=351.3 nm is only ₃1×10^–19 cm². Phase-matching occurred at concentrations of C_PM=0.0874 mol/dm³ in HFIP and 0.1088 mol/dm³ in TFE. A third-harmonic energy conversion efficiency of _E0.01 was achieved at a pump-laser peak intensity of I _0L2.5×10¹¹ W/cm² in a 5 mm long sample of PMC in TFE. The conversion efficiency is limited by destruction of phase-matching due to the intensity-dependent nonlinear refractive index of the dye solutions.     

Bounds on enhanced turbulent flame speeds for combustion with fractal velocity fields

Rigorous upper bounds are derived for large-scale turbulent flame speeds in a prototypical model problem. This model problem consists of a reaction-diffusion equation with KPP chemistry with random advection consisting of a turbulent unidirectional shear flow. When this velocity field is fractal with a Hurst exponentH with 0<H<1, the almost sure upper bounds suggest that there is an accelerating large-scale turbulent flame front with the enhanced anomalous propagation lawy=C _H t ^1+H for large renormalized times. In contrast, a similar rigorous almost sure upper bound for velocity fields with finite energy yields the turbulent flame propagation law within logarithmic corrections. Furthermore, rigorous theorems are developed here which show that upper bounds for turbulent flame speeds with fractal velocity fields are not self-averaging, i.e., bounds for the ensemble-averaged turbulent flame speed can be extremely pessimistic and misleading when compared with the bounds for every realization.     

Fine Structures of the Permittivity and Characteristic Losses of Electrons in Fluorite

Experimental-computational spectra of the permittivity and characteristic losses –Im^–1 for energies in the range 5–21 eV at a temperature of 4.2 K and theoretical spectra of and –Im^–1 of a fluorite crystal are resolved into elementary transition bands. The parameters of transition bands (energies of their maxima E _i, band halfwidths H _i and areas S _i, and oscillator forces f _i) are determined. A correlation of the spectral bands of and –Im^–1is established, and their specific features are elucidated.     

Frequency Dependent Conductivity of Thin ZnO Films Prepared by R.F. Sputtering Technique

AC conductivity of different thin zinc oxide films measured in the frequency range of 10 Hz to 2 MHz in the temperature interval of 300 K to 575 K is reported. ZnO films were prepared by reactive r.f. magnetron sputtering from ZnO target. The experimental data reveal that a.c. conductivity is proportional to ^s . The value of s was found to be temperature dependent, decreases with increasing temperature. These observations suggest that correlated barrier hopping model is the most likely mechanism. The temperature dependence of a.c. Conductivity is expressed in power law form as () T ⁿ . The temperature exponent n is found to be increasing with increasing temperature and decreasing frequency in accordance with the narrow band limit. At high temperature the conductivity variation with frequency is comparatively small. The polaron binding energy (W _m), the height of Coulomb barrier (W) and the characteristic relaxation time (₀) have been calculated. The values of W _m and W increase as the thickness decreases whereas the values of ₀ decrease with decreasing thickness.     

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     

Effects of OH concentration and temperature on NO emission characteristics of turbulent non-premixed CH4/NH3/air flames in a two-stage gas turbine like combustor at high pressure

This study examined the effects of OH concentration and temperature on the NO emission characteristics of turbulent, non-premixed methane (CH₄)/ammonia (NH₃)/air swirl flames in two-stage combustors at high pressure. Emission data were obtained using large-eddy simulations with a finite-rate chemistry method from model flames based on the energy fraction of NH₃ (E_NH3) in CH₄/NH₃ mixtures. Although NO emissions at the combustor exit were found to be significantly higher than those generated by CH₄/air and NH₃/air flames under both lean and stoichiometric primary zone conditions, these emissions could be lowered to approximately 300 ppm by employing far-rich equivalence ratios (?) of 1.3 to 1.4 in the primary zone. This effect was possibly due to the lower OH concentrations under far-rich conditions. An analysis of local flame characteristics using a newly developed mixture fraction equation for CH₄/NH₃/air flames indicated that the local temperature and NO and OH concentration distributions with local ? were qualitatively similar to those in NH₃/air flames. That is, the maximum local NO and OH concentrations appeared at local ? of 0.9, although the maximum temperature was observed at local ? of 1.0. Both the temperature and OH concentration were found to gradually decrease with the partial replacement of CH₄ with NH₃. Consequently, NO emissions from CH₄/NH₃ flames were maximized at E_NH3 in the range of 20% to 30%, after which the emissions decreased. Above 2100 K, the NO emissions from CH₄/NH₃ flames increased exponentially with temperature, which was not observed in NH₃/air flames because of the lower flame temperatures in the latter. But, the maximum NO concentration in CH₄/NH₃ flames was occurred at a temperature slightly below the maximum temperature, just as in NH₃/air flames. The apparent exponential increase in NO emissions from CH₄/NH₃ flames is attributed to a similar trend in the OH concentration at high temperatures.     

Zero value of the Schwarzschild mass for an asymptotically Euclidian system of gravitational waves

A class of the asymptotically Euclidian space-times is shown to exist for which the Schwarzschild mass is equal to zero. The coordinate atlases of these space-times satisfy two additional conditions: _k (-gg ^0k )=0 and _ik ⁰ _0g ^ik - _ik ^k _0g ⁰ⁱ =0. In aT-orthogonal metricgs ²=g ₀₀ dt ² -g dx dx these conditions take a simple form: ₀(detg )=0 and (₀ g )(₀ g )=0.     

Correlation inequalities for the truncated two-point function of an Ising ferromagnet

We establish the following new correlation inequalities for the truncated twopoint function of an Ising ferromagnet in a positive external field: _j ; _l ^T _j ; _k ^T _k ; _l ^T , and _j ; _l ^T _{k K j} ; _k ^T _{k l} , whereK is any set of sites which separatesj froml. The inequalities are also valid for the pure phases with zero magnetic field at all temperatures. Above the critical temperature they reduce to known inequalities of Griffiths and Simon, respectively.NSERC Postgraduate Fellow, 1978–1981. Research supported in part by NSF Grant No. PHY-78-25390-A02.     

Superradiating 4P-4S-3P cascade of sodium vapour arising on the leading edge of the exciting laser pulse

Investigations of the superradiating cascade of sodium vapour 4P-4S-3P ₁ = 2.21 µm and ₂=1.14 µm) arising on the leading edge of the exciting laser pulse were carried out. The dependences of the actual delay time _D of the ₁ pulse on the population rise time of the laser-excited 4P state were measured and compared with those calculated following the existing theoretical model. The dependence of the actual delay time _D on the inverse density of excited atoms 1/N* is also presented. Analysis of this dependence revealed the influence of the Doppler dephasing and of the second, ₂, transition on the formation of the ₁ superradiance.