Nitric oxide concentration measurements in atmospheric pressure flames using electronic-resonance-enhanced coherent anti-Stokes Raman scattering

We report the application of electronic-resonance-enhanced coherent anti-Stokes Raman scattering (ERE-CARS) for measurements of nitric oxide concentration ([NO]) in three different atmospheric pressure flames. Visible pump (532 nm) and Stokes (591 nm) beams are used to probe the Q-branch of the Raman transition. A significant resonance enhancement is obtained by tuning an ultraviolet probe beam (236 nm) into resonance with specific rotational transitions in the (v’=0, v”=1) vibrational band of the A²Σ⁺–X²Π electronic system of NO. ERE-CARS spectra are recorded at various heights within a hydrogen-air flame producing relatively low concentrations of NO over a Hencken burner. Good agreement is obtained between NO ERE-CARS measurements and the results of flame computations using UNICORN, a two-dimensional flame code. Excellent agreement between measured and calculated NO spectra is also obtained when using a modified version of the Sandia CARSFT code for heavily sooting acetylene-air flames (φ=0.8 to φ=1.6) on the same Hencken burner. Finally, NO concentration profiles are measured using ERE-CARS in a laminar, counter-flow, non-premixed hydrogen-air flame. Spectral scans are recorded by probing the Q₁ (9.5), Q₁ (13.5) and Q₁ (17.5) Raman transitions. The measured shape of the [NO] profile is in good agreement with that predicted using the OPPDIF code, even without correcting for collisional effects. These comparisons between [NO] measurements and predictions establish the utility of ERE-CARS for detection of NO in flames with large temperature and concentration gradients as well as in sooting environments. PACS 07.88.+y; 42.62.Fi; 42.65.Dr     

Effect of H-atom concentration on soot formation in premixed ethylene/air flames

Soot formation is a major challenge in the development of clean and efficient combustion systems based on hydrocarbon fuels. Fundamental understanding of the reaction mechanism leading to soot formation can be obtained by investigating the role of key reactive species such as atomic hydrogen taking part in soot formation pathways. In this study, two-dimensional laser induced incandescence (LII) measurements using λ?=?1064?nm laser have been used to measure soot volume fraction (f_V) in a series of rich ethylene (C₂H₄)/air flames, stabilized over a McKenna burner fitted with a flame stabilizing metal disc. Moreover, a comparison of UV (λ?=?283?nm), visible (λ?=?532?nm) and IR (λ?=?1064?nm) laser excited LII measurements of soot is discussed. Recently developed, femtosecond two-photon laser-induced fluorescence (fs-TPLIF) technique has been applied for obtaining spatially resolved H-atom concentration ([H]) profiles under the same flame conditions. The structure of the flames has also been determined using hydroxyl radical (OH) planar laser induced fluorescence (PLIF) imaging. The results indicate an inverse dependence of f_V on [H] for a range of C₂H₄/air rich flames up to an equivalence ratio, Φ?=?3.0. Although an absolute relationship between [H] and f_V cannot be easily derived owing to the multiple steps involving H and other intermediate species in soot formation pathways, the present study demonstrates the feasibility to couple [H] and f_V obtained using advanced optical techniques for soot formation studies.     

Femtosecond two-photon LIF imaging of atomic species using a frequency-quadrupled Ti:sapphire laser

Femtosecond (fs)-duration laser pulses are well suited for two-photon laser-induced-fluorescence (TPLIF) imaging of key atomic species such as H, N, and O in gas-phase reacting flows. Ultrashort pulses enable efficient nonlinear excitation, while reducing interfering photochemical processes. Furthermore, amplified fs lasers enable high-repetition-rate imaging (typically 1–10 kHz) for capturing the dynamics of turbulent flow fields. However, two-dimensional (2D), single-laser-shot fs-TPLIF imaging of the above species is challenging in most practical flow fields because of the limited ultraviolet pulse energy available in commercial optical parametric amplifier (OPA)-based tunable laser sources. In this work, we report the development of an efficient, fs frequency-quadrupling unit [i.e., fourth-harmonic generator (FHG)] with overall conversion efficiency more than six times greater than that of commercial OPA-based systems. The development, characterization, and application of the fs-FHG system for 2D imaging of H atoms in flames are described in detail. The potential application of the same laser system for 2D imaging of N and O atoms is also discussed.     

Capital budgeting and optimal timing of investments in flexible manufacturing systems

This paper investigates the financial-economic decision process for investments in flexible manufacturing systems (FMS). Contrary to popular belief, we show that conventional capital budgeting techniques can be used to make such investment decisions. First, we identify theoverall impact of installing an FMS and present guidelines for a cash flow forecasting model. We then present ways in which to incorporate uncertainty in these cash flows within a risk-adjusted discount rate. These expected cash flows and the discount rate are used in calculating the net present value (NPV). Once the capital budgeting analysis is completed, a critical issue facing the firm is the optimal timing of the installation. We reinterpret the general results on optimal timing of investments within the special context of an FMS project. Finally, we illustrate the above technique via a stylized example.     

Investigation of optical fibers for coherent anti-Stokes Raman scattering (CARS) spectroscopy in reacting flows

The objective of this work is to investigate the feasibility of intense laser-beam propagation through optical fibers for temperature and species concentration measurements in gas-phase reacting flows using coherent anti-Stokes Raman scattering (CARS) spectroscopy. In particular, damage thresholds of fibers, nonlinear effects during beam propagation, and beam quality at the output of the fibers are studied for the propagation of nanosecond (ns) and picosecond (ps) laser beams. It is observed that ps pulses are better suited for fiber-based nonlinear optical spectroscopic techniques, which generally depend on laser irradiance rather than fluence. A ps fiber-coupled CARS system using multimode step-index fibers is developed. Temperature measurements using this system are demonstrated in an atmospheric pressure, near-adiabatic laboratory flame. Proof-of-concept measurements show significant promise for fiber-based CARS spectroscopy in harsh combustion environments. Furthermore, since ps-CARS spectroscopy allows the suppression of non-resonant background, this technique could be utilized for improving the sensitivity and accuracy of CARS thermometry in high-pressure hydrocarbon-fueled combustors.     

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.     

One-dimensional single-shot thermometry in flames using femtosecond-CARS line imaging

We report single-laser-shot one-dimensional thermometry in flames using femtosecond coherent anti-Stokes Raman scattering (fs-CARS) line imaging. Fs-CARS enables high-repetition-rate (1-10?kHz), nearly collision-free measurement of temperature and species concentration in reacting flows. Two high-power 800?nm beams are used as the pump and probe beams and a 983?nm beam is used as the Stokes beam for CARS signal generation from the N2Q-branch transitions at ～2330?cm(-1). The probe beam is frequency-chirped for single-laser-shot imaging. All three laser beams are formed into sheets and crossed in a line which forms the probe region. The resulting 1D line-CARS signal at ～675?nm is spatially and spectrally resolved and recorded as a two-dimensional (2D) image. Single-shot temperature measurements are demonstrated in flat-field flames up to temperatures exceeding 2000?K, demonstrating the potential of fs-CARS line imaging for high-repetition-rate thermometry in turbulent flames. Such measurements can provide valuable data to validate complex turbulent-combustion models as well as increase the understanding of the spatio-temporal instabilities in practical combustion devices such as modern gas-turbine combustors and augmentors.     

Development of injection-seeded, pulsed optical parametric generator/oscillator systems for high-resolution spectroscopy

We report the development and application of pulsed optical parametric generator (OPG) and optical parametric oscillator (OPO) systems that are injection seeded with near-infrared distributed feedback diode lasers. The OPG is injection seeded at the idler wavelength without the use of a resonant cavity. Two counter-rotating, beta-barium-borate (β-BBO) crystals are used in the OPG. These crystals are pumped by the third harmonic, 355-nm output of an injection-seeded Nd:YAG laser. An OPO version of the system has also been developed by placing two flat mirrors around the two β-BBO crystals to form a feedback cavity at the signal wavelength. The OPO cavity length is not actively controlled. The output signal beam from the OPG or OPO is amplified using an optical parametric amplifier (OPA) stage with four β-BBO crystals. The frequency bandwidths of the signal and idler laser radiation from OPG/OPA and OPO/OPA systems have been determined to be slightly greater than 200 MHz. The temporal pulses from each system are smooth and near-Gaussian. High-resolution optical absorption measurements of acetylene (C₂H₂) were performed as another check of the frequency spectrum of the idler beam. The frequency-doubled signal output of the OPO/OPA system was used to perform high-resolution, single-photon, laser-induced fluorescence (LIF) spectroscopic studies of the (0,0) vibrational band of the A ²Σ⁺−X ²Π electronic transition of nitric oxide (NO) at low pressure. Excellent agreement was obtained between the theory and the experiment. The signal output of the OPG/OPA system was also used for sub-Doppler, two-photon LIF spectroscopic studies of the same vibration–rotation manifold of NO.This revised version was published online in August 2005 with a corrected cover date.     

Perturbative theory and modeling of electronic-resonance-enhanced coherent anti-Stokes Raman scattering spectroscopy of nitric oxide

A theory is developed for three-laser electronic-resonance-enhanced (ERE) coherent anti-Stokes Raman scattering (CARS) spectroscopy of nitric oxide (NO). A vibrational Q-branch Raman polarization is excited in the NO molecule by the frequency difference between visible Raman pump and Stokes beams. An ultraviolet probe beam is scattered from the induced Raman polarization to produce an ultraviolet ERE-CARS signal. The frequency of the ultraviolet probe beam is selected to be in electronic resonance with rotational transitions in the A (2)Sigma(+)<--X (2)Pi (1,0) band of NO. This choice results in a resonance between the frequency of the ERE-CARS signal and transitions in the (0,0) band. The theoretical model for ERE-CARS NO spectra has been developed in the perturbative limit. Comparisons to experimental spectra are presented where either the probe laser was scanned with fixed Stokes frequency or the Stokes laser was scanned with fixed probe frequency. At atmospheric pressure and an NO concentration of 100 ppm, good agreement is found between theoretical and experimental spectral peak locations and relative intensities for both types of spectra. Factors relating to saturation in the experiments are discussed, including implications for the theoretical predictions.