Spectroscopic,calibration and RET issues for linear laser-induced fluorescence measurements of nitric oxide in high-pressure diffusion flames

Two different strategies are compared for linear laser-induced fluorescence (LIF) measurements of nitric oxide concentration ([NO]) in counter-flow diffusion flames at high pressures via the A-X(0,0) system. Excitation of NO via a rovibronic transition at 226.03 nm is found to be slightly better compared to a previously utilized excitation wavelength of 225.58 nm. An indirect approach based on the computed spectral overlap fraction is verified and applied to calibrate [NO] measurements in counter-flow diffusion flames at high pressures. A five-level model for NO molecular dynamics is presented and utilized to investigate the effects of rotational energy transfer (RET) on linear LIF measurements of [NO] at pressures up to 15 atm. The results indicate that rotational relaxation effects are essentially negligible under high-pressure conditions at low laser fluences, and thus they need not be accounted for when measuring [NO] using linear LIF. The calibration technique is validated by direct comparisons to [NO] measurements made at pressures up to 5 atm via another calibration method, based on doping NO in counter-flow premixed flames at the same pressure. Using this calibration technique, LIF measurements of [NO] are obtained in a series of counter-flow diffusion flames at pressures up to 15 atm. These measurements are found to be in excellent agreement with previously reported measurements of [NO] in similar flames. PACS 07.35.+k; 33.20.Sn; 42.62.Fi     

Detection of trace nitric oxide concentrations using 1-D laser-induced fluorescence imaging

Spectrally resolved laser-induced fluorescence (LIF) with one-dimensional spatial imaging was investigated as a technique for detection of trace concentrations of nitric oxide (NO) in high-pressure flames. Experiments were performed in the burnt gases of premixed methane/argon/oxygen flames with seeded NO (15 to 50 ppm), pressures of 10 to 60 bar, and an equivalence ratio of 0.9. LIF signals were dispersed with a spectrometer and recorded on a 2-D intensified CCD array yielding both spectral resolution and 1-D spatial resolution. This method allows isolation of NO-LIF from interference signals due to alternative species (mainly hot O₂ and CO₂) while providing spatial resolution along the line of the excitation laser. A fast data analysis strategy was developed to enable pulse-by-pulse NO concentration measurements from these images. Statistical analyses as a function of laser energy of these single-shot data were used to determine the detection limits for NO concentration as well as the measurement precision. Extrapolating these results to pulse energies of ～?16 mJ/pulse yielded a predicted detection limit of ～?10 ppm for pressures up to 60 bar. Quantitative 1-D LIF measurements were performed in CH₄/air flames to validate capability for detection of nascent NO in flames at 10–60 bar.     

Temperature measurements of the gas-phase during surrogate diesel injection using two-color toluene LIF

Planar laser-induced fluorescence (LIF) of toluene has been applied in an optical engine and a high-pressure cell, to determine temperatures of fuel sprays and in-cylinder vapors. The method relies on a redshift of the toluene LIF emission spectrum with increasing temperature. Toluene fluorescence is recorded simultaneously in two disjunct wavelength bands by a two-camera setup. After calibration, the pixel-by-pixel LIF signal ratio is a proxy for the local temperature. A detailed measurement procedure is presented to minimize measurement inaccuracies and to improve precision. n-Heptane is used as the base fuel and 10 % of toluene is added as a tracer. The toluene LIF method is capable of measuring temperatures up to 700 K; above that the signal becomes too weak. The precision of the spray temperature measurements is 4 % and the spatial resolution 1.3 mm. We pay particular attention to the construction of the calibration curve that is required to translate LIF signal ratios into temperature, and to possible limitations in the portability of this curve between different setups. The engine results are compared to those obtained in a constant-volume high-pressure cell, and the fuel spray results obtained in the high-pressure cell are also compared to LES simulations. We find that the hot ambient gas entrained by the head vortex gives rise to a hot zone on the spray axis.     

UV planar laser induced fluorescence imaging of hot carbon dioxide in a high-pressure flame

UV planar laser-induced fluorescence (PLIF) images of hot carbon dioxide (CO₂) are obtained in a laminar flame (CH₄/air) at high pressure (20 bar) with excitation wavelengths at 239.34 nm and 242.14 nm. Excitation wavelengths are chosen to minimize the contribution of nitric oxide and molecular oxygen LIF signals. Spectrally resolved single point measurements are used for correction of the remaining oxygen LIF interference. The continuum LIF signal from electronically excited CO₂ is detected in a broad (280–400 nm) emission region. The UV PLIF of hot CO₂ has the potential for application to a wide variety of diagnostic needs in high-pressure flames, combustors, and engines. PACS 42.62.Fi; 42.30.Va; 07.25+k; 39.30+w     

New laser-induced fluorescence scheme for simultaneous OH and NO detection by a single laser set-up

In this communication, we propose a new laser-induced fluorescence (LIF) scheme that allows the simultaneous detection of OH and NO by a single laser set-up. OH is detected by the second harmonic (SH) of a dye laser tuned to the (0,0)-band of the 3064 ? system, while its third harmonic (TH) is used to detect NO through excitation of the (2,0)-band of the γ system. This scheme is presented and discussed within the framework of its potential use in field instruments for the measurement of tropospheric OH concentration. Received: 8 March 2002 / Revised version: 22 April 2002 / Published online: 8 August 2002     

Planar laser-induced fluorescence imaging of carbon monoxide using vibrational (infrared) transitions

We report a new imaging diagnostic suitable for measurements of infrared-active molecules, namely infrared planar laser-induced fluorescence (IR PLIF), in which a tunable infrared source is used to excite vibrational transitions in molecules and vibrational fluorescence is collected by an infrared camera. A nanosecond-pulse Nd:YAG-pumped KTP/KTA OPO/OPA system is used to generate 12 mJ of tunable output near 2.35 μm which excites the 2ν band of carbon monoxide (CO); fluorescence resulting from excited CO is collected at 4.7 μm by using an InSb focal plane array. Quantitative, high-SNR PLIF imaging of gas-phase CO is demonstrated at a 10-Hz acquisition rate with a minimum detection limit of 1350 ppm at 300 K. Received: 30 July 1999 / Published online: 16 September 1999     

Detailed measurements of transient two-stage ignition and combustion processes in high-pressure spray flames using simultaneous high-speed formaldehyde PLIF and schlieren imaging

This study investigates the low- and high-temperature ignition and combustion processes in a high-pressure spray flame of n-dodecane using simultaneous 50-kHz formaldehyde (HCHO) planar laser-induced fluorescence (PLIF) and 100-kHz schlieren imaging. The PLIF measurements were facilitated through the use of a pulse-burst-mode Nd:YAG laser, producing a 355-nm pulse-train with 300 pulses at 70 mJ/pulse, separated by 20-µs, in a 6-ms burst. The high-speed HCHO PLIF signal was imaged using a non-intensified CMOS camera with dynamic background emission correction. The acquisition rate of this HCHO PLIF diagnostic is unique to the research community, and when combined with high-speed schlieren imaging, provides unprecedented opportunity for analysis of the spatiotemporal evolution of fuel jet penetration and low- and high-temperature ignition processes relevant to internal combustion engine conditions. The present experiments are conducted in the Sandia constant-volume preburn vessel equipped with a new Spray A injector. The influences of ambient conditions are examined on the ignition delay times of the two-stage ignition events, HCHO structures, and lift-off length values. Consistent with past studies of traditional Spray A flames, the formation of HCHO is first observed in the jet peripheries where the equivalence ratio (Φ) is expected to be leaner and hotter and then grows in size and in intensity downstream into the jet core where Φ is expected to be richer and colder. The measurements demonstrate that the formation and propagation of HCHO from the leaner to richer region leads to high-temperature ignition events, supporting the identification of a phenomenon coined “cool-flame wave propagation” during the transient ignition process. Subsequent high-temperature ignition is found to consume the previously formed HCHO in the jet head, while the formation of HCHO persists in the fuel-rich zone near the flame base over the entire combustion period.     

Temperature measurement in fuel-rich non-sooting low-pressure hydrocarbon flames

Several temperature measurement techniques were compared for the investigation of fuel-rich, premixed, flat, low-pressure flames of propene, acetylene, and cyclopentene with maximum temperatures around 2400 K. Vibrational Stokes/anti-Stokes Raman measurements with a KrF excimer laser using CO, H₂, and H₂O as temperature indicators were examined at 50 and 200 mbar for different flame stoichiometries. Also, laser-induced fluorescence (LIF) of OH in the A-X band was used, and complementary lifetime measurements were performed to account for a variation of fluorescence quantum yield with rotational quantum number. LIF using seeded NO (0.2-1.0%) was applied both in point-wise and 1D temperature measurement in spite of the anticipated interaction of NO with the fuel-rich flame chemistry. Furthermore, thermocouple measurements were performed in the preheat zone. These techniques were compared with respect to accuracy and the potential for routine applications under fuel-rich low-pressure conditions.     

Experimentally based correction procedures for planar laser-induced fluorescence measurements of mean species concentration

Experimentally-based correction procedures are demonstrated which enhance the quantitative nature of planar laser-induced fluorescence (PLIF) images for mean species concentration by correcting for the influence of the electronic quenching rate coefficient. Implementation of these methods requires only the ability to make PLIF and laser-saturated fluorescence (LSF) measurements. Though applied herein to NO, these procedures are broadly applicable both in terms of species and users. Moreover, they are generally effective regardless of the error gradients associated with spatial variations in the electronic quenching rate coefficient. In such general environments, these methods produce quenching-corrected, spatially resolved PLIF images of mean species concentration with a total uncertainty equivalent to that of a single LSF measurement. Received: 22 November 1999 / Revised version: 3 March 2000 / Published online: 16 June 2000     

Gas-phase temperature imaging in spray systems using multi-line NO-LIF thermometry

Two-dimensional gas-phase temperature fields were measured in spray flames and evaporating spray systems using laser-induced fluorescence (LIF) of nitric oxide (NO). The recently developed multi-line technique yields absolute temperature without calibration. It is successfully applied to temperature measurements in the presence of droplets. The method is based on the temperature dependence of the NO-LIF signal. Measurements have been carried out in heated nitrogen flows at room temperature to validate the accuracy (<±1%) and precision (1%) of the technique by comparing results to thermocouple readings. Temperature measurements in a dilute evaporating acetone spray at room temperature showed cooling of the entrained air of 15±6 K. Temperature imaging in an ethanol spray flame at various conditions yields the entire temperature range from the coflow temperature at 300±4 K (1%) to the flame temperature at 1900±40 K (2%). PACS 07.20.Dt; 32.50.+d; 42.62.Fi     

Quantitative dual-tracer planar laser-induced fluorescence measurements of molecular mixing

Simultaneous, planar laser-induced fluorescence (LIF) images of nitric oxide (NO) and acetone have been used to calculate instantaneous quantitative maps of molecularly mixed jet-fluid fraction in an axisymmetric shear layer. In this experiment, NO is seeded into high-purity nitrogen jet fluid and acetone is seeded into air coflow. On mixing at the molecular level, the NO LIF is strongly quenched by oxygen from the coflow, while the acetone signal is unaffected by the mixing process. The extent to which the jet fluid is mixed at the molecular level is determined on a pixel-by-pixel basis from the simultaneous NO and acetone planar LIF images. Jets at Reynolds numbers ranging from 1000 to 50 000 are investigated.     

Toluene laser-induced fluorescence for in-cylinder temperature imaging in internal combustion engines

A single-laser single-camera imaging technique was demonstrated for in-cylinder temperature distribution measurements in a direct-injection internal combustion engine. The single excitation wavelength two-color detection technique is based on toluene laser-induced fluorescence (LIF). Toluene-LIF emission spectra show a red-shift with increasing temperature. Temperature can thus be determined from the ratio of the signal measured in two separate wavelength ranges independent of the local tracer concentration, laser pulse energy, and the intensity distribution. An image doubling and filtering system is used for the simultaneous imaging of two wavelength ranges of toluene LIF onto the chip of a single camera upon excitation at 248 nm. The measurements were performed in a spark-ignition engine with homogeneous charge and yielded temperature images with a single-shot precision of approximately ±?6%.     

NO and PO photofragments as trace analyte indicators of nitrocompounds and organophosphonates

Laser photolysis that releases characteristic photofragments, combined with laser-induced fluorescence (LIF) that subsequently monitors them, facilitate detection of trace-vapor analytes in air. The feasibility of the technique is demonstrated for nitrocompounds and organophosphonates detection. Using one-color and two-color lasers, respectively, the representative NO and PO photofragments were tagged. Employment of longer wavelengths for photodissociation, and where possible also for LIF, than for fluorescence collection, obstructs background fluorescence and in the former compounds also prevents interference of ambient ground state NO. Received: 1 February 2000 / Revised version: 27 April 2000 / Published online: 20 September 2000     

Evolution and impingement of an automotive fuel spray investigated with simultaneous Mie/LIF techniques

The spatial and temporal evolution of an automotive hollow-cone-type spray was investigated with laser-based imaging diagnostics. Optical conditions of an IC engine were emulated with a test cell that was built from an engine cylinder head to hold a high-pressure gasoline-fuel injector. The use of iso-octane fuel that was doped with 3-pentanone allowed measurements of laser-induced fluorescence (LIF) after excitation with a KrF excimer-laser beam. A versatile optical filter system was designed and built that permits simultaneous measurements of Mie-scattering and laser-induced-fluorescence images using a single laser-light sheet and a single intensified CCD camera. The influence of background signals, caused by reflection of signal light from surfaces, laser-sheet intensity attenuation and signal decrease by scattering, was characterized. Mass distributions showed a distinct pre-spray phase, more so than the Sauter mean diameter (SMD) that was determined from the ratio of LIF to Mie signals using single pulse as well as averaged image pairs. Significant changes in SMD distributions were found after the spray had impinged on a flat surface. The impingement also led to the buildup of a liquid film whose thickness was quantitatively determined from LIF images. Received: 5 December 2000 / Revised version: 28 February 2001 / Published online: 23 May 2001     

Attenuation corrections for in-cylinder NO LIF measurements in a heavy-duty Diesel engine

Quantification of the nitric oxide (NO) concentration inside the cylinder of a Diesel engine by means of laser-induced fluorescence (LIF) measurements requires, amongst others, knowledge of the attenuation of the ultraviolet radiation involved. We present a number of laser diagnostic techniques to assess this attenuation, enabling a correction for laser intensity and detection efficiency of the raw NO LIF data. Methods discussed include overall laser beam transmission, bidirectional laser scattering (bidirectional LIF), spectrally resolved fluorescence imaging, and Raman scattering by N₂. A combination of techniques is necessary to obtain the complete attenuation of laser beam and NO fluorescence. The overall laser beam transmission measurements and bidirectional LIF measurements (the latter yielding spatially resolved transmission) provide evidence of a non-uniform attenuation distribution, with predominant attenuation within or near the piston bowl. Fluorescence imaging of multiple vibrational bands through a spectrograph is shown to be a powerful method for obtaining spatially resolved data on the transmission losses of fluorescence. Special attention is paid to the role of CO₂ and O₂ as UV light absorbers, and the consequences to different excitation-detection schemes for NO. PACS 82.33.Vx; 42.62.Fi; 33.20.t     

Characterization of ammonia two-photon laser-induced fluorescence for gas-phase diagnostics

Two-photon laser-induced fluorescence (LIF) of ammonia (NH₃) with excitation of the C′-X transition at 304.8 nm and fluorescence detection in the 565 nm C′-A band has been investigated, targeting combustion diagnostics. The impact of laser irradiance, temperature, and pressure has been studied, and simulation of NH₃-spectra, fitted to experimental data, facilitated interpretation of the results. The LIF-signal showed quadratic dependence on laser irradiance up to 2 GW/cm². Stimulated emission, resulting in loss of excited molecules, is induced above 10 GW/cm², i.e., above irradiances attainable for LIF imaging. Maximum LIF-signal was obtained for excitation at the 304.8 nm bandhead; however, lower temperature sensitivity over the range 400–700 K can be obtained probing lines around 304.9 nm. A decrease in fluorescence signal was observed with pressure up to 5 bar absolute and attributed to collisional quenching. A detection limit of 800 ppm, at signal-to-noise ratio 1.5, was identified for single-shot LIF imaging over an area of centimeter scale, whereas for single-point measurements, the technique shows potential for sub-ppm detection. Moreover, high-quality NH₃-imaging has been achieved in laminar and turbulent premixed flames. Altogether, two-photon fluorescence provides a useful tool for imaging NH₃-detection in combustion diagnostics.     

Point and planar ultraviolet excitation/detection of hydroxyl-radical laser-induced fluorescence through long optical fibers

We demonstrate an all-fiber-coupled, UV, laser-induced-fluorescence (LIF) detection system of the hydroxyl radical (OH) in flames. The nanosecond-pulsed excitation of the (1,0) band of the OH A(2)∑(+)-X(2)Π system at ～283 nm is followed by fluorescence detection from the (0,0) and (1,1) bands around 310 nm. The excitation-laser beam is delivered through a 400 μm core UV-grade optical fiber of up to 10 m in length, and the fluorescence signal collected is transmitted through a 1.5 mm core 3 m long fiber onto the remote detector. Single-laser-shot planar LIF (PLIF) imaging of OH in flames is also demonstrated using fiber-based excitation. The effects of delivering intense UV beams through long optical fibers are investigated, and the system improvements for an all-fiber-coupled OH-PLIF imaging system are discussed. Development of such fiber-based diagnostics and imaging systems constitutes a major step in transitioning laser diagnostic tools from research laboratories to reacting flow facilities of practical interest.     

Fluorescence quantum yield of carbon dioxide for quantitative UV laser-induced fluorescence in high-pressure flames

The fluorescence quantum yield for ultraviolet laser-induced fluorescence of CO₂ is determined for selected excitation wavelengths in the range 215–250 nm. Wavelength-resolved laser-induced fluorescence (LIF) spectra of CO₂, NO, and O₂ are measured in the burned gases of a laminar CH₄/air flame (φ=0.9 and 1.1) at 20 bar with additional NO seeded into the flow. The fluorescence spectra are fit to determine the relative contribution of the three species to infer an estimate of fluorescence quantum yield for CO₂ that ranges from 2–8×10^?6 depending on temperature and excitation wavelength with an estimated uncertainty of ±0.5×10^?6. The CO₂ fluorescence signal increases linearly with gas pressure for flames with constant CO₂ mole fraction for the 10 to 60 bar range, indicating that collisional quenching is not an important contributor to the CO₂ fluorescence quantum yield. Spectral simulation calculations are used to choose two wavelengths for excitation of CO₂, 239.34 and 242.14 nm, which minimize interference from LIF of NO and O₂. Quantitative LIF images of CO₂ are demonstrated using these two excitation wavelengths and the measured fluorescence quantum yield.     

Simultaneous laser-induced fluorescence and sub-Doppler polarization spectroscopy of the CH radical

The first application of polarization spectroscopy (PS) to the CH radical is demonstrated. In particular, we report on the simultaneous application of laser-induced fluorescence (LIF) and sub-Doppler PS to CH. The conventional experimental setup for PS was supplemented with a second detection system in order to collect the LIF emission. At the same time a Fabry–Perot etalon and molecular iodine were utilized to obtain a precise relative and absolute frequency scale, respectively. CH was investigated in a low pressure methane–oxygen flame. The R₂(5) transition of the B–X (0, 0) band corresponding to a wavelength around 387.3 nm was scanned while fluorescence emission was collected in the spectral region around 431 nm from the B–X (0, 1), A–X (1, 1) and A–X (0, 0) bands. The saturation behavior of both techniques is investigated as well as line broadening effects due to the pump laser pulse energy or rather fluence. Saturation fluence for LIF was found to be more than one order of magnitude higher as compared to PS.     

Measurement of water film thickness by laser-induced fluorescence and Raman imaging

We present two non-intrusive, laser-based imaging techniques for the quantitative measurement of water fluid film thickness. The diagnostics methods are based on laser-induced fluorescence (LIF) of the organic tracer ethyl acetoacetate added to the liquid in sub-percent (by mass) concentration levels, and on spontaneous Raman scattering of liquid water, respectively, both with excitation at 266 nm. Signal intensities were calibrated with measurements on liquid layers of known thickness in a range between 0 and 500 μm. Detection via an image doubler and appropriate filtering in both light paths enabled the simultaneous detection of two-dimensional liquid film thickness information from both methods. The thickness of water films on transparent quartz glass plates was determined with an accuracy of 9% for the tracer LIF and 15% for the Raman scattering technique, respectively. The combined LIF/Raman measurements also revealed a preferential evaporation of the current tracer during the time-resolved recording of film evaporation.