Hydroxyl tagging velocimetry in a supersonic flow over a cavity

Hydroxyl tagging velocimetry (HTV) measurements of velocity were made in a Mach 2 (M 2) flow with a wall cavity. In the HTV method, ArF excimer laser (193 nm) beams pass through a humid gas and dissociate H2O into H + OH to form a tagging grid of OH molecules. In this study, a 7 x 7 grid of hydroxyl (OH) molecules is tracked by planar laser-induced fluorescence. The grid motion over a fixed time delay yields about 50 velocity vectors of the two-dimensional flow in the plane of the laser sheets. Velocity precision is limited by the error in finding the crossing location of the OH lines written by the excimer tag laser. With a signal-to-noise ratio of about 10 for the OH lines, the determination of the crossing location is expected to be accurate within +/- 0.1 pixels. Velocity precision within the freestream, where the turbulence is low, is consistent with this error. Instantaneous, single-shot measurements of two-dimensional flow patterns were made in the nonreacting M 2 flow with a wall cavity under low- and high-pressure conditions. The single-shot profiles were analyzed to yield mean and rms velocity profiles in the M 2 nonreacting flow.     

Hydroxyl tagging velocimetry method optimization: signal intensity and spectroscopy

The previously demonstrated nonintrusive time-of-flight molecular velocity tagging method, hydroxyl tagging velocimetry (HTV), has shown the capability of operating both at room temperature and in flames. Well-characterized jets of either air (nonreacting cases) or hydrogen-air diffusion flames (reacting cases) are employed. A 7 x 7 OH line grid is generated first through the single-photon photodissociation of H2O by a approximately 193 nm pulsed narrowband ArF excimer laser and is subsequently revealed by a read laser sheet through fluorescence caused by A2sigma+(v' = 3) <-- X2pi(i)(v' = 0), A2sigma+(v' = 1) <-- X2pi(i)(v' = 0), or A2sigma+(v' = 0) < or = X2pi(i)(v' = 0) pumping at approximately 248, approximately 282, or approximately 308 nm, respectively. A detailed discussion of the spectroscopy and relative signal intensity of these various read techniques is presented, and the implications for optimal HTV performance are discussed.     

Picosecond planar laser-induced fluorescence measurements of OH A 2 + ( ' = 2) lifetime and energy transfer in atmospheric pressure flames

A picosecond, excimer-Raman laser (268 nm, 400 ps FWHM) was used for laser sheet excitation of OH in the (2, 0) band. The fluorescence was detected with a fast-gated, intensified camera (400-ps gate width). The effective collisional lifetime of the spectrally integrated fluorescence was measured in two dimensions by shifting the intensifier gate across the decay curve. The average lifetime is ~2.0 ns for a stoichiometric methane -air flame with spatial variations of +/-10 %. Shorter collisional lifetimes were measured for rich flame conditions that are due to a higher number density of the quenchers. Vibrational energy transfer (VET) was observed in premixed methane -air and methane -oxygen flames by putting the fast-gated camera behind a spectrometer. The spectrum of the methane -air flame shows strong VET in contrast with the methane -oxygen flame. This is because N2 is a weak electronic quencher but a strong VET agent. By fitting the measured time dependence of the different vibrational populations ( ' = 2, 1, 0) to a four-level model, rate constants for quenching and VET were determined. For the lower states ( ' = 0, 1) our results are in good agreement with literature values. For a prediction of a spectrally integrated, collisional lifetime in a known collisional environment it is important to consider not only the quenching but also the amount of energy transfer in the excited state as well as the spectral detection sensitivity.     

Quantitative hydroxyl concentration time-series measurements in turbulent nonpremixed flames

Quantitative hydroxyl concentration time-series measurements have been obtained by picosecond time-resolved laser-induced fluorescence in a series of methane-air and hydrogen-argon-air nonpremixed flames. The recovery of a quantitative time series is complicated by the need to account for fluctuations in the fluorescence lifetime. We have recently developed instrumentation that enables the simultaneous measurement of fluorescence signal and lifetime. The present research represents the first application of this technique to turbulent flames. The correction for hydroxyl lifetime fluctuations is shown to be significant for mean concentrations and thus probability density functions but negligible for power spectral densities (PSD's). The hydroxyl PSD's were found to vary slightly with radial and axial location in the flames and to vary significantly with Reynolds number. However, the PSD's in the H(2)-Ar-air flames are nearly identical to those in the CH(4)-air flames.     

Measurements of CO, CO2, OH, and H2O in room-temperature and combustion gases by use of a broadly current-tuned multisection InGaAsP diode laser

A new laser technology that achieves nearly 100-nm quasi-continuous tuning with only injection-current control in a four-section grating-coupler sampled-reflector laser was used to detect CO and CO(2) simultaneously in room-temperature gas mixtures. The same grating-coupler sampled-reflector laser was used to perform in situ measurements of CO, H(2)O, and OH in the exhaust gases of a CH(4)-air flame. This laser is being evaluated for inclusion in a multispecies combustion-emissions exhaust-analysis sensor, and its operational characteristics as they have an impact on gas sensing are described. Preliminary results suggest that this single laser can be used to replace multilaser sensor configurations for some combustion-emissions monitoring applications.     

Line Raman, Rayleigh, and laser-induced predissociation fluorescence technique for combustion with a tunable KrF excimer laser

We have applied a line UV Raman, Rayleigh, and laser-induced predissociation fluorescence technique for measurement of turbulent hydrocarbon flames. The species concentration of CO(2), O(2), CO, N(2), CH(4), H(2)O, OH, and H(2) and the temperature are measured instantaneously and simultaneously along a line of 11.4 mm, from which the gradients with respect to mixture fraction and spatial direction are obtained. The technique has been successfully tested in a laminar premixed stoichiometric methane flame and a laminar hydrogen diffusion flame. In addition the technique has been tested in a highly turbulent rich premixed methane flame. The data show that the technique can be used to provide instantaneous measurements of local profiles that describe the local flame structure in highly turbulent flames.     

One-Dimensional, Time-Resolved Raman Measurements in a Sooting Flame made with 355-nm Excitation

Single-shot vibrational Raman measurements were performed along an 11-mm-long line crossing the reaction zone in a premixed, fuel-rich (phi = 10), laminar methane-air flame by use of a frequency-tripled Nd:YAG laser with a 355-nm emission wavelength. This laser source seems to have advantages relative to KrF excimer lasers as well as to Nd:YAG lasers at 532 nm for hydrocarbon combustion diagnostics. The Raman emissions of all major species (N(2), O(2), CH(4), H(2), CO(2), H(2)O) were detected simultaneously with a spatial resolution of 0.4 mm. By integration over selected spectral intervals, the mole fractions of all species and subsequently the local gas temperatures have been obtained. A comparison of the temperatures that were found with results from filtered Rayleigh experiments showed good agreement, indicating the success of what are to the best of our knowledge the first one-dimensional single-shot Raman measurements in a sooting hydrocarbon flame.     

Comparison of nanosecond and picosecond excitation for interference-free two-photon laser-induced fluorescence detection of atomic hydrogen in flames

Two-photon laser-induced fluorescence (TP-LIF) line imaging of atomic hydrogen was investigated in a series of premixed CH4/O2/N2, H2/O2, and H2/O2/N2 flames using excitation with either picosecond or nanosecond pulsed lasers operating at 205 nm. Radial TP-LIF profiles were measured for a range of pulse fluences to determine the maximum interference-free signal levels and the corresponding picosecond and nanosecond laser fluences in each of 12 flames. For an interference-free measurement, the shape of the TP-LIF profile is independent of laser fluence. For larger fluences, distortions in the profile are attributed to photodissociation of H2O, CH3, and/or other combustion intermediates, and stimulated emission. In comparison with the nanosecond laser, excitation with the picosecond laser can effectively reduce the photolytic interference and produces approximately an order of magnitude larger interference-free signal in CH4/O2/N2 flames with equivalence ratios in the range of 0.5< or =Phi< or =1.4, and in H2/O2 flames with 0.3< or =Phi< or =1.2. Although photolytic interference limits the nanosecond laser fluence in all flames, stimulated emission, occurring between the laser-excited level, H(n=3), and H(n=2), is the limiting factor for picosecond excitation in the flames with the highest H atom concentration. Nanosecond excitation is advantageous in the richest (Phi=1.64) CH4/O2/N2 flame and in H2/O2/N2 flames. The optimal excitation pulse width for interference-free H atom detection depends on the relative concentrations of hydrogen atoms and photolytic precursors, the flame temperature, and the laser path length within the flame.     

Generation of 224-nm radiation by stimulated Raman scattering of ArF excimer laser radiation in a mixture of H2 and D2

Raman shifting of tunable ArF excimer laser radiation in a mixture of H(2) and D(2) produces tunable radiation in the 224-nm region as a result of Stokes shifting the frequency of the fundamental radiation (193 nm) once in both H(2) and D(2). At a total pressure of 25 bars, a 19% H(2) in D(2) mixture is found to provide a maximum conversion efficiency (2.5%) to the 224-nm range. Both fundamental and 224-nm radiation were used to record laser-induced fluorescence excitation spectra of nitric oxide produced in an oxyacetylene flame. From the excitation spectra, we determined the tuning range of the 224-nm radiation to be 270 cm(-1) with a linewidth of 0.9 cm(-1), which is similar to the fundamental laser radiation. We derived the exact Raman shift of the generated radiation by comparing both excitation spectra which was found to be 7142.3(5) cm(-1).     

Simultaneous vibrational and pure rotational coherent anti-stokes Raman spectroscopy for temperature and multispecies concentration measurements demonstrated in sooting flames

The potential of measuring temperature and multiple species concentrations (N2, O2, CO) by use of combined vibrational coherent anti-Stokes Raman spectroscopy (CARS) and pure rotational CARS has been investigated. This was achieved with only one Nd:YAG laser and one dye laser together with a single spectrograph and CCD camera. From measurements in premixed sooting C2H4-air flames it was possible to evaluate temperatures from both vibrational CARS and rotational CARS spectra, O2 concentration from the rotational CARS spectra, and CO concentration from the vibrational CARS spectra. Quantitative results from premixed sooting C2H4-air flames are presented, and the uncertainties in the results as well as the possibility of extending the combined CARS technique for probing of additional species are discussed.     

Application of 266-nm and 355-nm Nd:YAG laser radiation for the investigation of fuel-rich sooting hydrocarbon flames by raman scattering

We describe the use of linear Raman scattering for the investigation of fuel-rich sooting flames. In comparison, the frequency-tripled and -quadrupled fundamental wavelengths of a Nd:YAG laser have been used as an excitation source for study of the applicability of these laser wavelengths for analysis of sooting flames. The results obtained show that, for the investigation of strongly sooting flames, 266-nm excitation is better than 355-nm excitation. Although the entire fluorescence intensity of polycyclic aromatic hydrocarbons (PAHs) decreases with rising excitation wavelength, there is increased interference with the Raman signals by displacement of the spectral region of the Raman signals toward the fluorescence maximum of the laser-induced fluorescence emissions. Besides the broadband signals of PAHs, narrowband emissions of laser-produced C2 occur in the spectra of sooting flames and affect the Raman signals. These C2 emission bands are completely depolarized and can be separated by polarization-resolved detection. A comparison of the laser-induced fluorescence emissions of an ethylene flame with those of a methane flame shows the same spectral features, but the intensity of the emissions is larger by a factor of 5 for the ethylene fuel. Using 266-nm radiation for Raman signal excitation makes possible measurements in the ethylene flame also.     

Two-Line Laser-Induced Fluorescence Imaging of Vibrational Temperatures in a NO-Seeded Flame

Two-dimensional temperature fields are measured in lean and sooting flames by means of two-color laser-induced fluorescence (LIF) imaging that uses seeded NO. Vibrational thermometry is performed by the probing of different vibrational ground-state levels. Spectral properties of the excited transitions within the A (2)?(+)-X (2)? system are well known from previous studies. The energy difference of 1974 cm(-1) between the (0, 0)Q(1) + P(21)(33.5) and the (0, 2)O(12)(5.5) lines offers great sensitivity in the temperature range that is relevant for combustion processes. Excitation is possible by use of a tunable KrF excimer laser on its fundamental (248-nm) and Raman shifted (in H(2), 225-nm) wavelengths. An excitation scheme for instantaneous two-line measurements by use of a single laser is developed. The possibility of single-shot measurements is discussed.     

Quantitative imaging of temperature and OH in turbulent diffusion flames by using a single laser source

We describe a diagnostic technique for obtaining quantitative, simultaneous, and instantaneous images of temperature and the concentration of the hydroxyl radical OH in turbulent flames. The technique uses a single laser source and a single intensified CCD camera. A stoichiometric premixed flame is used for calibration. We use detailed calculations of laminar flames of similar fuels to estimate the effects of quenching and ground-state population on the OH signal. A factor combining both effects is generated as a function of temperature. We validate the technique by comparing measured temperature and OH number density with calculated values in laminar diffusion flames. Absolute errors of 10-20% and 20-30% are estimated on the measured temperature and OH number density, respectively. The technique is applicable to regions of the flames where the Rayleigh cross section is close to that of air.     

Two-point time-series measurementsof hydroxyl concentration in a turbulent nonpremixed flame

Quantitative two-point hydroxyl time-series measurements have been performed in a turbulent nonpremixed flame by using two-point picosecond time-resolved laser-induced fluorescence. The current diagnostic system has been improved from its preliminary version to address optical aberrations and fluorescence lifetime fluctuations. In particular, with a newly designed collection system, the aberration-limited blur spot is reduced from 6 mm to 180 microm. Additional photon-counting channels enable the recovery of absolute OH concentrations through a triple-bin integration method. The present research represents what we believe to be the first application of this two-point technique to turbulent flames. Two independent schemes have been applied to remove uncorrelated noise in the derived two-point statistics. We show that optical aberrations can have a significant effect on space-time correlations. However, the sampling rate and fluctuations in the fluorescence lifetime barely affect the spatial autocorrelation function and thus the integral length scale. Such length scales for hydroxyl are found to rise linearly with increasing axial distance at peak [OH] locations. Along the jet centerline, the integral length scale varies slightly below the flame tip but increases rapidly above the flame tip. In addition, the OH length scale demonstrates the same trend as the OH time scale along the jet centerline, but the opposite trend at peak [OH] locations.     

Improving signal-to-interference ratio in rich hydrocarbon-air flames using picosecond coherent anti-Stokes Raman scattering

There is growing interest in the use of short-pulse lasers for coherent anti-Stokes Raman scattering (CARS) to minimize non-resonant background (NRB) contributions in a variety of applications. Using time-coincident picosecond (ps) pump and Stokes beams and a time-delayed ps probe beam, we show that a three orders of magnitude reduction in NRB interference can be achieved in rich hydrocarbon-air flames while preserving 60% to 80% of the CARS signal. This represents a significant improvement in signal-to-interference ratio compared with previous measurements in room temperature air and is attributable to reduced rates of collisional dephasing and relaxation at flame temperatures. Measurements within the flame zone of a laminar flat-flame burner are used to investigate the characteristics of time-coincident and probe-delayed broadband ps N(2)-CARS spectra for C(2)H(4)-air equivalence ratios of 0.5 to 1.2. Up to three ro-vibrational bands of N(2) are excited with each laser shot using 135 ps pump and 106 ps Stokes beams, and the CARS signal is generated using a 135 ps probe beam delayed by 165 ps. The enhanced signal-to-interference ratio achieved in the current work is one to two orders of magnitude higher than that previously achieved using polarization-selection techniques without sensitivity to the effects of birefringence caused by density gradients or test cell windows. Moreover, the use of a 135 ps laser source in this study enables frequency domain "broadband" CARS with sufficient resolution to extract ro-vibrational spectral features under various flame conditions. The effect of probe delay and NRB suppression on characteristics of these broadband CARS spectra are investigated, and evidence of preferential collisional dephasing and relaxation of different ro-vibrational transitions is not detected. This is a promising but preliminary result to be investigated further in future work.     

Quantitative technique for imaging mixture fraction, temperature, and the hydroxyl radical in turbulent diffusion flames

A technique for obtaining simultaneous quantitative images of the hydroxyl radical, OH, temperature, mixture fraction, and scalar dissipation rates in turbulent diffusion flames is described. Mixture fraction is obtained from images of Rayleigh and fuel Raman scattering. We quantified the OH laser-induced fluorescence (LIF) images using detailed calibration and a correction for quenching and population distribution effects based on the simultaneous mixture fraction and temperature images. This correction was derived from calculations of laminar counterflow diffusion flames for identical fuel mixtures. These laminar flame computations are further used to estimate the errors in the measured OH concentrations. The technique is applied to piloted, nonpremixed flames over a range of jet velocities. The measured mixture fraction, temperature, and OH concentrations are in good agreement with those obtained earlier in similar flames using the single-point Raman/Rayleigh/LIF technique.     

Visualization of CN by the use of planar laser-induced fluorescence in a cross section of an unseeded turbulent CH(4)-air flame

CN is known to be the important species in forming NO(x) in hydrocarbon-air flames, and we describe the qualitative mapping of the CN distribution of the order of less than 1 in 10(6) at atmospheric pressure in a cross section of an unseeded turbulent CH(4)-air flame by the use of a single-shot laser pulse with planar laser-induced fluorescence. We obtained the results by comparing the different excitation-detection schemes to find the most appropriate scheme for visualization. In addition, the images obtained have good spatial resolution of 200 μm. Based on a laminar flame experiment with the same optical systems, it is observed that the CN distribution zone is located outside of the inner cone even at atmospheric pressure.     

Laser-induced predissociative fluorescence: dynamics and polarization and the effect of lower-state rotational energy transfer on quantitative diagnostics

Laser-induced predissociative fluorescence is often used for diagnostics because its short-lived upper states are minimally disturbed by collisions. We discuss the effects of lower-state collisions with parameters relevant to our atmospheric H(2)-O(2) flame. A pulse of tunable KrF excimer-laser light induces the A ? X, Q(1)(11), 3 ? 0 transition in OH. We measure the intensity and the polarization of the resulting A ? X, Q(1)(11), 3 ? 2 fluorescence as a function of laser brightness. A simple model that uses no adjustable parameters produces a reasonable fit to the data. It predicts that, even at very modest laser energies, the fluorescence intensity is almost directly proportional to the rate constant for rotational energy transfer (RET) within the lower vibrational state. That rate constant can be a strong function of local conditions. Furthermore, under typical operating conditions the excimer will pump an amount of OH out of the lower state that is many times as large as that originally present. This occurs because RET within the X-state continuously replenishes the lower state during the laser pulse. Even when this occurs, the signal may still vary linearly with laser intensity, and the polarization may be nearly that expected for weak pumping. At the higher laser intensities, a significant fraction of the measured OH arises from two-photon photodissociation of the water from the flame reaction.     

Temperature measurement by degenerate four-wave mixing with strong absorption of the excitation beams

We have made simultaneous temperature measurements by degenerate four-wave mixing (DFWM) and absorption spectroscopy of OH in a CH(4)-air, lifted-diffusion flame. After we corrected the DFWM data for laser beam absorption of as much as 60%, the DFWM-based temperatures were in good agreement with temperatures derived strictly from the absorption data, as well as a one-dimensional reacting flow simulation.     

Phase-locked two-line OH planar laser-induced fluorescence thermometry in a pulsating gas turbine model combustor at atmospheric pressure

Two-line OH planar laser-induced fluorescence (PLIF) thermometry was applied to a swirling CH4/air flame in a gas turbine (GT) model combustor at atmospheric pressure, which exhibited self-excited combustion instability. The potential and limitations of the method are discussed with respect to applications in GT-like flames. A major drawback of using OH as a temperature indicator is that no temperature information can be obtained from regions where OH radicals are missing or present in insufficient concentration. The resulting bias in the average temperature is addressed and quantified for one operating condition by a comparison with results from laser Raman measurements applied in the same flame. Care was taken to minimize saturation effects by decreasing the spectral laser power density to a minimum while keeping an acceptable spatial resolution and signal-to-noise ratio. In order to correct for the influence of laser light attenuation, absorption measurements were performed on a single-shot basis and a correction procedure was applied. The accuracy was determined to 4%-7% depending on the location within the flame and on the temperature level. A GT model combustor with an optical combustion chamber is described, and phase-locked 2D temperature distributions from a pulsating flame are presented. The temperature variations during an oscillation cycle are specified, and the general flame behavior is described. Our main goals are the evaluation of the OH PLIF thermometry and the characterization of a pulsating GT-like flame.