Comparison of laser-induced and planar laser-induced fluorescence measurements of nitric oxide in a high-pressure, swirl-stabilized, spray flame

We report spatially resolved linear laser-induced fluorescence (LIF) and planar laser-induced fluorescence (PLIF) measurements of nitric oxide (NO) in a pre-heated, high-pressure (4.27 atm), lean direct-injection (LDI) spray flame. The feasibility of using PLIF in lieu of LIF is assessed with respect to measuring NO concentrations in high-pressure LDI spray flames. NO is excited via the resonant Q₂(26.5) transition of the γ(0,0) band while a non-resonant wavelength is employed to subtract background interferences. LIF detection is performed in a 2-nm region centered on the γ(0,1) band. PLIF detection is performed in a 68-nm window that captures fluorescence from several vibrational bands. An in situ NO doping scheme for fluorescence calibration is successfully employed to quantify the LIF signals. However, a similar calibration scheme for the reduction of PLIF images to quantitative field measurements is plagued by the laser-excited background. Excitation scans and calibration comparisons have been performed to assess the background contribution for PLIF detection. Quantitative radial NO profiles measured by LIF are presented and analyzed so as to correct the PLIF measurements to within the accuracy bars of the LIF measurements via a single-point scaling of the PLIF image. Received: 23 November 1999 / Revised version: 17 January 2000 / Published online: 27 April 2000     

The use of rovibrationally excited NO photofragments as trace nitrocompounds indicators

A one-color laser performs photolysis of nitrocompounds and laser-induced fluorescence to monitor the generated NO photofragments and to sensitively detect vapor trace amounts of nitrocompounds. The NO is monitored via excitation and emission through A²Σ⁺(v^′=0)?X²Π(v^′′=2-0) and A²Σ⁺(v^′=0)?X²Π(v^′′=0,1) transitions, respectively. It is found that NO photofragments populate the vibrationless ground state and also the first two vibrationally excited states. The analytical performance of the method is demonstrated on 2,4 dinitrotoluene (DNT) via excitation through A²Σ⁺(v^′=0)?X²Π(v^′′=2). The achieved limits of detection are 3.7 and 2.7 parts per billion (ppb) by weight of gaseous DNT in 100 and 500 Torr of air, for 30 s integration time. The application of this scheme for trace nitrocompound detection has the advantage that no background of ambient ground-state NO interferes and that the fluorescence is collected at shorter wavelengths than the exciting radiation, precluding background fluorescence. Received: 18 August 1999 / Revised version: 22 November 1999 / Published online: 8 March 2000     

Laser diagnostics of NO reburning in fuel-rich propene flames

Absolute NO concentrations were measured by laser-induced fluorescence (LIF) in three different fuel-rich non-sooting propene flames (φ=1.5, 1.8 and 2.3). The experiments were performed in low-pressure premixed propene flames with 0.2%-1% NO added. Laser diagnostics was applied as a tool for investigating reburn chemistry. The Q₂(25.5) line in the A-X(0,0) band was excited because of the small temperature dependence of its ground state population. The NO fluorescence lifetimes were measured directly and compared to theoretical values. The initial NO levels are strongly reduced in all three flames. According to modeling results, the HCN mole fraction increases strongly with stoichiometry. As guidelines for laser diagnostics applications in such systems, the modeling results were analyzed with respect to the main reaction channels and reaction partners in fuel-rich flames. Received: 1 March 2000 / Revised version: 20 April 2000 / Published online: 20 September 2000     

Photochemical effects of KrF excimer excitation in laser-induced fluorescence measurements of OH in combustion environments

This paper presents experimental evidence that using the KrF excimer laser for quantitative laser-induced fluorescence (LIF) studies of the OH A-X (3,0) system is highly problematic if the effects of both photobleaching and photochemistry are not included for laser spectral irradiances greater than 20 MW/cm² cm^-1. Pump-probe and time-resolved measurements of the OH LIF signal in an atmospheric pressure, premixed CH₄-air flame at low- and high-laser-spectral-irradiance conditions show that a significant amount of OH is produced from photofragments resulting from the simultaneous 2-photon predissociation of H₂O molecules in the C-X system. A 5+2-level rate-equation model that includes the effects of both photobleaching and photochemical OH production is shown to satisfactorily predict the data using a single adjustable parameter given by the effective, spectrally integrated 2-photon cross-section of H₂O near 248 nm. The time-integrated OH LIF signal was found to depend on both the laser spectral irradiance and the local concentration of H₂O. Additionally, use of the KrF excimer laser for 2-line rotational thermometry can produce temperature errors as great as +550 K at high laser-pulse energies. Received: 21 August 2000 / Revised version: 30 October 2000 / Published online: 21 February 2001     

Laser-diagnostic multi-species imaging in strongly swirling natural gas flames

Within the TECFLAM group a standard swirl burner is investigated, both experimentally using optical and probe measurements and by simulations using different modeling attempts. The present study is focused on the laser-based investigation of the NO distribution within the reacting flow field of a strongly swirling, confined 150-kW natural gas flame. Simultaneous quantitative measurements of NO- and OH-concentration fields by laser-induced fluorescence imaging (LIF) and temperature distribution (Rayleigh scattering) are performed. Mixing properties of the unburned gases are investigated for the isothermal and the combusting flow using tetrahydrothiophene (THT) as a new fluorescing tracer. These measurements show which areas are sufficiently mixed allowing for the application of planar Rayleigh thermometry. Areas where THT-LIF interferes with OH-LIF detection are localized and omitted from data evaluation. The data is analyzed yielding global scalar fields for comparison with model simulations and correlations between the different measured scalars are investigated showing an almost linear correlation of NO concentration and temperature within the swirl flame whereas no apparent correlation between NO and OH concentration was found. Received: 20 April 2000 / Revised version: 16 May 2000 / Published online: 20 September 2000     

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     

燃烧产物组成激光诱导荧光光谱的测量

对激光诱导荧光（LIF）光谱技术在燃烧过程中的应用进行研究，介绍测量燃烧过程中常见自由基OH和NO的LIF光谱的实验方案，以及采用激光诱导荧光光谱技术测量小分子荧光光谱的方法，利用YAG激光器、染料激光器、CO2激光器、光谱仪、ICCD等设备对燃烧产物中常见小分子自由基OH和NO进行了测量，从实验中得到了自由基OH和NO的荧光光谱。实验结果表明，荧光光谱与激发波长无关，但是激发波长改变后，荧光强度因离开最佳波长而有所下降，这符合分子荧光光谱的特征。与其他光谱技术相比，激光诱导荧光光谱技术具有极高的选择性和灵敏度。     

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     

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.     

Raman-Rayleigh-LIF measurements of temperature and species concentrations in the Delft piloted turbulent jet diffusion flame

We report a series of Raman-Rayleigh-LIF measurements in two turbulent natural-gas jet diffusion flames produced by the Delft piloted jet diffusion flame burner. The main objective of the Raman-Rayleigh-LIF measurements was to obtain detailed information on the major species concentrations in the flames. The measurements provide simultaneous data on temperature, the concentrations of the major species and the radicals OH and NO and mixture fraction. The application of the Raman technique in the undiluted natural-gas flames proves to be very challenging because of the high fluorescence interference levels. The interference contributions to the recorded Raman signals are identified and subtracted using empirical correlations between the Raman signals and the signals on fluorescence interference monitor channels. The calibration and data reduction of the Raman-Rayleigh and LIF signals are discussed in detail. The resulting dataset compares excellently with data from previous experiments. Because the Raman-Rayleigh-LIF data provide quantitative concentrations and accordingly quantitative mixture fractions, they form a valuable and useful extension of the existing database for the Delft piloted jet diffusion flame burner. Received: 19 October 1999 / Revised version: 31 January 2000 / Published online: 7 June 2000     

Quantitative, dynamic fuel distribution measurements in combustion-related devices using laser-induced fluorescence imaging of biacetyl in iso-octane

Knowledge of in-situ fuel distributions in practical combustion devices, such as internal combustion engines, is crucial for research and devlopment purposes. Numerous imaging techniques, mostly based on laser-induced fluorescence (LIF), have been developed and yield high levels of 2-D spatial information, but generally lack the temporal resolution (frame rates) necessary to resolve important timescales at sub-millisecond levels for sustained times. A planar LIF technique for quantitatively visualizing fuel distribution is presented which gives not only high spatial resolution, but also high temporal resolution. Using a high-speed CMOS camera, a lens-coupled image intensifier, and frequency-tripled diode-pumped Nd:YAG laser allows for capturing LIF images of biacetyl that is used as a fluorescence tracer at 12 kHz (one crank-angle resolution at 2000 RPM) for hundreds of consecutive engine cycles. The LIF signal strength of biacetyl doped in iso-octane is shown to vary substantially over a wide range of temperatures and pressures. The low absorption coefficient at 355 nm and a longpass filter in the detection path exclude bias errors due to laser beam attenuation and fluorescence trapping. An intensifier gate time of 350 ns is shown to suppress the detection of phosphorescence signals under practical conditions. An example for a quantitative high-speed measurement of fuel concentration at varying pressure and temperature conditions is presented. Quantitative equivalence ratio maps are shown for the fuel injection event within a single cycle in a spark-ignition direct-injected engine, showing the ability of the technique to not only reveal static fuel concentration maps, but also the motion of the fuel cloud along with very steep gradients. Spray velocities determined from the moving fuel cloud are in agreement with previous particle image velocimetry measurements.     

NO激光诱导荧光对高焓气流温度的测量

由于真实气体效应,高超声速流场的研究仍然依赖于大量的实验.流场温度是实验的重要参数,目前只能通过具有非入侵性质的光学测量手段获得,然而,由于多方面的难题,鲜有对高焓流场参数测量的报道.文章介绍了利用激光诱导荧光（laser-induced fluorescence,LIF）技术对JF-10氢氧爆轰激波风洞产生的高焓实验气流温度的测量工作.搭建了用于脉冲式风洞的LIF测量系统,使用了NO分子作为荧光组分.因为高焓流场实验条件苛刻,本实验对传统的激光设置进行了调整,使用了平行于拍摄方向的竖直平面激光激发NO,使荧光信号更为集中,获得了清晰的LIF图像.利用双线测温法（two-line thermometry,TLT）测量高焓自由流中NO分子的转动温度,从而确定气流的平转温度.测量结果表明,JF-10实验气流的平转温度为600 K.      

土壤有机污染物激光诱导荧光光谱检测方法研究进展

土壤有机物污染源广、危害程度高、监测手段有限,是继水污染、大气污染又一个引起全球关注的环境问题。土壤有机污染快速在线检测分析对农业生产、土壤调查、土质修复有着重要的意义。激光诱导荧光(LIF)光谱技术是一种基于光致发光的物质成分和含量分析技术,具有样品使用量少、预处理过程简单、检测速度快等特点,在环境科学、生物分析、生命科学等众多领域有广泛应用。国内外研究人员展开大量研究工作,已形成较完善的方法体系及技术设备。文章介绍了LIF测量系统的组成结构和工作原理,综述了现阶段LIF技术在土壤有机污染物检测研究进展,重点包括土壤中油类污染物、多环芳烃污染物、有机农药污染物的识别及定量分析方法等,以及仪器开发过程中涉及的相关问题,给出了LIF技术在土壤有机污染物检测方面的发展趋势,为进一步发展基于LIF技术的土壤有机污染物现场快速检测仪器提供参考。     

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     

Simultaneous multiple-line Raman/Rayleigh/LIF measurements in combustion

It is demonstrated that multiple 1D Raman scattering, Rayleigh scattering, and laser-induced fluorescence (LIF) measurements can be performed simultaneously. This can be used for quasi-2D (or quasi-3D) single-shot measurements of multiple species and the temperature in turbulent reacting and non-reacting flows. The technique has the potential to yield more precise information than most competitive planar imaging approaches in combustion. For example, it can be used to overcome Raman/LIF interference problems in technical flames. This is achieved by a new optical set-up that makes use of an imaging spectrograph combined with fiber optics. Received: 13 October 1999 / Revised version: 26 November 1999 / Published online: 27 January 2000     

Measurements and simulation of in-cylinder UV-absorption in spark ignition and Diesel engines

Spatially and spectrally resolved in-cylinder absorption measurements were performed in spark-ignited internal combustion engines and in Diesel engines. With UV-broadband illumination it was shown that the UV attenuation occurs throughout the burned gas area with roughly homogeneous absorption cross-sections. Model calculations based on the absorption properties of CO₂ at elevated temperatures show that this species gives the main contribution to in-cylinder UV absorption. A previously suggested technique of assessing UV absorption using O₂ laser-induced fluorescence (LIF) as probe light is successfully applied to in-cylinder measurements of the light absorption inside a fired heavy-duty Diesel engine. Even in this environment, the comparison with model calculations shows that CO₂ is the main contributor to UV light absorption. Since the O₂-LIF absorption technique is based on the identical geometry used for LIF concentration measurements, the results can directly be used for correcting LIF signal data such as that obtained from NO imaging. Received: 20 April 2001 / Published online: 18 July 2001     

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     

Spatially resolved absolute concentration and fluorescence-lifetime determination of H2CO in atmospheric-pressure CH4/air flames

Using laser-induced fluorescence (LIF), spatially resolved concentration profiles of formaldehyde (H₂CO) were obtained in the preheating zone of atmospheric-pressure premixed CH₄/air flames stabilized on the central slot of a multiple-slot burner similar in construction to domestic boilers. The isolated pQ₁(6) rotational line (339.23 nm) in the 2¹ ₀4¹ ₀ vibronic combination transition in the ?¹A₂- ¹A₁ electronic band system around 339 nm was excited in the linear LIF intensity regime. For a quantification of quenching effects on the measured LIF signal intensities, relative fluorescence quantum yields were determined from direct fluorescence lifetime as a function of height above the slot exit. Absolute H₂CO number densities in the flames were evaluated from a calibration of measured LIF signal intensities versus those obtained in a low-pressure sample with a known H₂CO vapor pressure. Peak concentrations in the slightly lean and rich flames reached (994±298) and (174±52) ppm, respectively. Received: 25 September 2000 / Published online: 30 November 2000     

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.     

Experimental evaluation of strategies for quantitative laser-induced-fluorescence imaging of nitric oxide in high-pressure flames (1-60 bar)

Nitric oxide laser-induced-fluorescence (NO-LIF) 2-D imaging measurements using a new multi-spectral detection strategy are reported for high-pressure flames (1-60 bar). This work builds on previous research that identified interference LIF from O₂ and CO₂ in high-pressure flames and optimized the choice of excitation strategies as a function of application conditions. In this study, design rules are presented to optimize the LIF detection wavelengths for quantitative 2-D NO-LIF measurements over a wide range of pressures (1-60 bar) and temperatures. Simultaneous detection of LIF in multiple wavelength regions enables correction of the NO signal for interference from O₂ and CO₂ and allows simultaneous imaging of all three species. New experiments of wavelength-resolved 1-D LIF in slightly lean (? = 0.9) and slightly rich (? = 1.1) methane/air flames are used to evaluate the design rules and estimate the NO detection limits for a wide range of flame conditions. The quantitative 2-D measurements of NO in the burnt gas are compared with model calculations (using GRI-Mech 3.0) versus pressure for slightly lean and slightly rich flames. The discussions and demonstrations reported in this study provide a practical guideline for application of instantaneous 1-D or 2-D NO-LIF imaging strategies in high-pressure combustion systems.