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     

ps-LIF measurements of minor species concentration in a counterflow diffusion flame interacting with a vortex

Interactions of vortices and flame fronts may be considered as the basic structural elements of turbulent combustion. Additionally, they play an important role in flame instabilities as well as extinction and ignition processes. An ideal geometry to study these interactions is the counterflow diffusion burner with an additional actuator-driven nozzle for the generation of a vortex ring. This burner has already been well-characterized by other methods including CARS, LDA and PLIF. We present first quantitative measurements of minor species concentration in this flame using a short-pulse laser and time- and spatially resolved fluorescence detection with a streak camera. Quench-free OH concentrations are obtained by analysis of the time-resolved profiles. The high power density of the laser pulses allowed linewise detection of hydrogen using a three-photon excitation scheme. Simultaneously, shape and position of the vortex was monitored using two-dimensional detection of flame emissions. Spatially resolved concentration profiles of H and OH are presented for different interaction heights and times in the vortex. For steady flames, comparisons with model calculations are shown. Received: 19 July 2000 / Revised version: 13 December 2000 / Published online: 21 February 2001     

Flame growth and wrinkling in a turbulent flow

High-speed planar laser-induced fluorescence (PLIF) and 3-D large eddy simulations (LES) are used to study turbulent flame kernel growth, wrinkling and the formation of separated flame pockets in methane/air mixtures. Turbulence was effected by a set of rotary fans situated in a cylindrical enclosure. Flame wrinkling was followed on sequential 2-D OH images captured at kHz repetition rates. Under stoichiometric conditions and low turbulence levels the flame kernel remains singly connected and close to spherical in shape. By increasing turbulence or reducing the stoichiometry of the mixture the formation of separated pockets could be observed and studied. The mechanisms behind these phenomena are investigated qualitatively by LES of a level-set G-equation describing the flame surface propagation in turbulent flows. Received: 12 April 2000 / Revised version: 26 June 2000 / Published online: 5 October 2000     

Pressure and composition dependences of acetone laser-induced fluorescence with excitation at 248, 266, and 308 nm

In previous studies, acetone has been successfully applied as a tracer for planar laser-induced fluorescence (PLIF) measurements of concentration and temperature. The desire to extend acetone PLIF capability to conditions of varying pressure and composition has motivated studies of the effects of these quantities on fluorescence yield. The present work explores pressure and composition effects over a 0.5 to 16 atm range for the three excitation wavelengths of greatest interest for diagnostics: 248, 266, and 308 nm. In accord with previous studies, fluorescence per acetone molecule is seen to increase with pressure, apparently towards a high-pressure limit for each wavelength, with the most significant effect observed at short wavelengths. Bath gas composition is also seen to affect fluorescence intensity, with an impact related to the effectiveness of the bath gas species at vibrationally relaxing excited acetone. A model of fluorescence yield considering the relative rates of intersystem crossing and vibrational relaxation for excited singlet acetone describes the measured pressure and composition dependences well. To explain an oxygen fluorescence quenching effect that is observed experimentally, a term is added to the model to represent oxygen-assisted intersystem crossing. The data and model results provide useful guidance for diagnostic applications. A key conclusion is that long excitation wavelengths are preferable from the standpoint of minimizing pressure and composition dependences. Received: 17 December 1998 / Revised version: 21 May 1999 / Published online: 30 July 1999     

Measurement of temperature, fuel concentration and equivalence ratio fields using tracer LIF in IC engine combustion

A technique based on planar laser-induced fluorescence of 3-pentanone, for measurements of absolute concentration, temperature and fuel/air equivalence ratios in turbulent, high-pressure combustion systems such as an internal combustion engine is presented. Quasi-simultaneous excitation with 248 nm and 308 nm of 3-pentanone that is used as a fluorescence tracer doped to iso-octane, yields pairs of strongly temperature-dependent fluorescence images. Previous investigations have resulted in information on temperature and pressure dependence of absorption cross-sections and fluorescence quantum yields. Using these data the ratio of corresponding fluorescence images can be converted to temperature images. Instantaneous temperature distribution fields in the compression stroke and in the unburned end-gas of an SI engine were measured. The temperature fields obtained from the two-line technique are used to correct the original tracer-LIF images in order to evaluate quantitative fuel distributions in terms of number densities and fuel/air equivalence ratio. Received: 10 March 2000 / Revised version: 19 April 2000 / Published online: 16 August 2000     

Quasi-simultaneous detection of CH2O and CH by cavity ring-down absorption and laser-induced fluorescence in a methane/air low-pressure flame

The combination of two-dimensional, planar laser-induced fluorescence (PLIF) and cavity ring-down (CRD) absorption spectroscopy is applied to map quantitatively the spatial distributions of CH₂O and CH in a methane/air flame at 25 Torr. Both species are detected in the same spectral region using the overlapping CH₂O A ¹ A ₂ -X ¹ A ₁ 4₁ ⁰ and CH B-X(1,0 )bands. The combination of diagnostic techniques exploits the spatial resolution of LIF and the quantitative CRD absorption measure of column density. The spatially resolved PLIF provides the distribution of absorbers and line-of-sight CRD absorption the absolute number density needed for quantitative concentration images. The peak CH₂O concentration is (3.5±1.4 )×10¹⁴ cm^-3, or 1450±550 ppm at 1000 K. The lack of precise absorption cross-section data produces these large error limits. Although a flame model predicts lower amounts, these large uncertainties limit this measurement’susefulness as a test of the flame chemistry. Received: 24 April 2001 / Revised version: 10 July 2001 / Published online: 10 October 2001     

Analysis of the local conformation of proteins with two-dimensional fluorescence techniques

Two 2D fluorescence techniques are described which allow the study of conformational changes in proteins in their native form in μM solutions using aromatic amino acids (tryptophan, tyrosine) as intrinsic fluorescence markers. Simultaneous time- and wavelength-resolved fluorescence spectra are measured using a 80 ps laser source in conjunction with streak detection in the exit plane of an astigmatism-corrected spectrometer. This approach allows identification of different photophysical processes by their associated lifetime and spectral intensity distribution; errors due to the more common integration over a wider spectral range are avoided. Time-resolved spectra are sensitive to changes in the collisional environment (dynamic quenching) and can thus be used to monitor local conformation changes close to the respective fluorophors. This is demonstrated for the Ras protein which undergoes a drastic conformation change while binding to different nucleotides. Excitation-emission spectra are two-dimensional fluorescence images with one axis corresponding to the excitation and the other to the emission wavelength. Thus, they contain all conventional excitation and fluorescence spectra of a given substance. The 2D structure facilitates the interpretation of these spectra and allows the direct identification of resonance effects, scattering and the isolation of the contribution of different fluorophors to the complete spectrum. This is demonstrated for mixtures of tyrosine and tryptophan. In this case, both wavelength-resolved spectra and temporal decays are affected by energy transfer processes between the two amino acids. In a last example, both static and time-resolved spectral methods are combined to determine the respective contribution of static and dynamic quenching in calsequestrin. Evaluation of the fluorescence data is in good agreement with a recent crystallographic analysis which shows that all tryptophans are located in a conserved domain of the protein. Addition of Ca²⁺ ions leads to a more compact form of calsequestrin and to polymers. This information would not be obtainable from either of the two techniques alone. Received: 10 February 2000 / Published online: 13 September 2000     

Cs(6P)+(Ne,N2)碰撞能量转移

在气体样品池条件下,研究了Cs(6P3/2) (Ne,N2)碰撞能量转移过程.用调频半导体激光器激发Cs原子至Cs(6P3/2)态,在不同的Ne或N2气压下,测量了直接6P3/2→6S1/2荧光和转移6P1/2→6S1/2荧光,对于6P3/2与Ne的碰撞,电子态能量仅能转移为Ne原子的平动能.在与N2的碰撞中,向分子振转态的转移是重要的.利用速率方程分析,可以得到碰撞转移速率系数,对于Ne,6PJ精细结构碰撞转移速率系数为1.45×10-12cm3·s-1.对于N2,测量6P Ne和6P N2二种情况下荧光的相对强度比,确定精细结构速率系数为1.64×10-12cm3·s-1,6P态猝灭速率系数为4.88×10-12cm3·s-1.     

Comparison of techniques for non-intrusive fuel drop size measurements in a subscale gas turbine combustor

In aviation gas turbine combustors, many factors, such as the degree and extent of fuel/air mixing, and fuel vaporization achieved prior to combustion, influence the formation of pollutants. To assist in analyzing the extent of fuel/air mixing, flow visualization techniques have been used to interrogate the fuel distributions during subcomponent tests of lean-burning fuel injectors. Combustor pressures (up to 14 bar) and air inlet temperatures (up to 680K) were typical of actual gas turbine engine operating conditions. Discrimination between liquid and vapor phases of the fuel was accomplished by comparing planar laser-induced fluorescence (PLIF) images, elastically-scattered light images, and phase/Doppler interferometer measurements. Estimates of Sauter mean diameters are made by ratioing PLIF and Mie scattered intensities for various sprays, and factors affecting the accuracy of these estimates are discussed. Mie calculations of absorption coefficients indicate that the droplet fluorescence intensities are proportional to their surface areas, instead of their volumes, due to the high absorbance of the liquid fuel for the selected excitation wavelengths.     

Sustained simultaneous high-speed imaging of scalar and velocity fields using a single laser

A high-speed technique that combines planar laser induced fluorescence (PLIF) detection of biacetyl and particle image velocimetry (PIV) for simultaneous imaging of scalar and velocity fields is demonstrated at a frame rate of 12 kHz for up to 32500 consecutive frames. A single diode-pumped, frequency-tripled Nd-YAG laser was used for excitation. Wavelength-separated recording was achieved for Mie scattering from silicone oil droplets with a CMOS camera and for the red-shifted fluorescence from biacetyl with an image-intensified CMOS camera. Interference between PIV and PLIF tracers was found to be negligible. Cross-talk between PIV and PLIF signals was low and a strategy to completely eliminate it was devised and is discussed. The signal-to-noise ratio is about 9 for single-shot scalar images. Example image sequences were recorded in an atmospheric pressure air jet at Re=2000. PACS 42.62.Fi; 33.50.Dq; 06.30.Gv; 06.60.Jn     

Temperature and excitation wavelength dependencies of 3-pentanone absorption and fluorescence for PLIF applications

The temperature and excitation wavelength dependencies of 3-pentanone absorption and fluorescence were studied in support of planar laser-induced fluorescence (PLIF) imaging of temperature and mixture fraction in flows of practical interest. The temperature dependencies (300–875 K) of absorption and fluorescence were measured for gaseous 3-pentanoneat atmospheric pressure in a nitrogen bath gas using 248, 266, and 308 nm excitation. The results indicate that the fluorescence signal per unit mole fraction using 248 nm excitation is highly temperature-sensitive below 600 K, while the signal from 308 nm excitation is not temperature sensitive below 500 K. For quantitative measurements over a broad range of temperatures, one must choose excitation schemes carefully to balance the trade-off between measurement sensitivity and the amount of signal at the expected conditions. As an example of such a choice and to show the capabilities of ketone PLIF techniques, we include temperature and mixture fraction images of a 300–650 K heated air jet using near-simultaneous 308 and 266 nm excitation. Received: 29 May 2002 / Revised version: 5 November 2002 / Published online: 26 February 2003 RID="*" ID="*"Corresponding author. Fax: +1-650/723-1748, E-mail: jkoch@stanford.edu RID="**" ID="**"E-mail: hanson@me.stanford.edu     

Wide- and narrow-band saturated fluorescence measurements of hydroxyl concentration in premixed flames from 1 bar to 10 bar

We have studied the use of wide-band detection in conjunction with saturation of a rovibronic transition of OH within itsA ^{2 +}–X ²(0,0) band. For wide-band detection, in which fluorescence is detected from the entire excited rotational manifold, the fluorescence yield is sensitive to collisions in two ways. First, it is sensitive to the ratio of rate coefficients describing rotational energy transfer and electronic quenching; this ratio determines the number of neighboring rotational levels that are populated during the laser pulse. Second, the fluorescence yield can vary with the total collisional rate coefficient; only after a sufficient number of collisions, corresponding to 2.5 ns in an atmospheric flame, does the rotational manifold reach steady state. We also compare measurements employing wide-band (detecting theR ₁ andR ₂ branches) and narrow-band (detecting a single transition) saturated fluorescence of OH. Over a wide range of conditions — obtained by varying the equivalence ratio, temperature, N₂ dilution, and pressure — the wide- and narrow-band fluorescence techniques compare well. Given this good agreement, wide-band saturated fluorescence could be especially useful for analyzing atmospheric flames with XeCl-excimer lasers; one can potentially obtain 2—D images of OH which have a high signal-to-noise ratio and a reduced sensitivity to laser irradiance and quenching.     

Fluorescence methods for detecting the kinetics of photosensitizer release from nanosized carriers

Three approaches to analyzing the rate of release of the photosensitizer meta-tetrahydroxyphenylchlorin (mTHPC) from unilaminar lipid vesicles (ULV) in model biological systems are studied: by excitation energy transfer from probe diphenylhexatriene to mTHPC, by the fluorescence anisotropy of mTHPC, and by photoinduced quenching of the fluorescence of mTHPC. Each of these methods has its characteristic range of sensitivity for measurements of the local concentration of mTHPC in ULV. Fluorescence anisotropy can be used for quantitative determination of the mTHPC yield from ULV for mTHPC:lipid ratios of 1:100 to 1:1000, determining the efficiency of fluorescence quenching of diphenylhexatriene for ratios <1:200, and photoinduced quenching for ratios of 1:10–1:500.     

Rb(5PJ)与He,N2的碰撞精细结构混合和猝灭

在气体样品池条件下,研究了Rb(5PJ) (He,N2)碰撞能量转移过程.用调频半导体激光器激发Rb原子至Rb(5P3/2)态,在不同的He或N2气压下,测量了直接5P3/2→5S1/2荧光和转移5P1/2→5S1/2荧光.对于Rb(5PJ)与He的碰撞,只发生精细结构转移(略去碰撞猝灭效应),电子态能量仅能转移为He原子的平动能.在与N2的碰撞中,向分子振转态的转移是重要的.本实验中,Rb的密度为4.5×1011 cm-3,由辐射陷获理论得到5P1/2→5S1/2的有效辐射率为2.47×107 s-1.利用速率方程分析,可以得到碰撞转移速率系数,对于He,5P3/2→5S1/2转移速率系数kHe21=2.61×10 12 cm3·s.对于N2,测量5PJ He和5PJ N2两种情况下直接荧光与敏化荧光的相对强度比,利用最小二乘法确定5Pa/2→5S1/2转移速率系数kN212=2.36×10-11 cm3·s,5PJ态猝灭速率系数kN2=1.44×10-11 cm3·s-1.由实验结果证实了Cs-N2主要是直线式碰撞传能机制,与其他实验结果进行了比较.     

Fluorescence quantum yield of rhodamine 101 in the presence of absorption saturation

Using the photothermal method we measure the fluorescence quantum yield of a rhodamine 101 solution in ethanol for different values of the pump-field fluence. Our experiments reveal a depletion of the fluorescence quantum yield as the pump fluence increases. To explain the observed fluorescence quenching, a dependence of the nonradiative relaxation rates on the field fluence is proposed. Predictions of the model are in good agreement with the experiments. Received: 16 November 1999 / Revised version: 5 July 2000 / Published online: 13 September 2000     

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     

High-speed CH planar laser-induced fluorescence imaging using a multimode-pumped optical parametric oscillator

We report on high-speed CH planar laser-induced fluorescence (PLIF) imaging in turbulent diffusion flames using a multimode-pumped optical parametric oscillator (OPO). The OPO is pumped by the third-harmonic output of a multimode Nd:YAG cluster for direct signal excitation in the A-X (0,0) band of the CH radical. The lasing threshold, conversion efficiency, and linewidth are shown to depend on the number of pump passes in the ring cavity of the OPO. Single-shot CH PLIF images are acquired at 10 kHz with excitation energy up to 6 mJ/pulse at 431.1 nm. Signal-to-noise ratios of ~25-35 are the highest yet reported for high-speed CH PLIF.     

Quantitative NO-LIF imaging in high-pressure flames

Planar laser-induced fluorescence (PLIF) images of NO concentration are reported in premixed laminar flames from 1–60 bar exciting the A-X(0,0) band. The influence of O₂ interference and gas composition, the variation with local temperature, and the effect of laser and signal attenuation by UV light absorption are investigated. Despite choosing a NO excitation and detection scheme with minimum O₂-LIF contribution, this interference produces errors of up to 25% in a slightly lean 60 bar flame. The overall dependence of the inferred NO number density with temperature in the relevant (1200–2500 K) range is low (<±15%) because different effects cancel. The attenuation of laser and signal light by combustion products CO₂ and H₂O is frequently neglected, yet such absorption yields errors of up to 40% in our experiment despite the small scale (8 mm flame diameter). Understanding the dynamic range for each of these corrections provides guidance to minimize errors in single shot imaging experiments at high pressure. Received: 13 May 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