Stability Analysis of the Fluorescent Tracer 1-Methylnaphthalene for IC Engine Applications by Supercontinuum Laser Absorption Spectroscopy.

1-methylnaphthalene (1-MN) is a widely used laser-induced fluorescence (LIF) tracer for planar imaging of mixture formation and temperature distributions in internal combustion (IC) engines. As the LIF measurement results can be biased by partial tracer oxidation, the conversion of 1-MN and the base fuel isooctane is analyzed in a calibration cell. First, measurements using supercontinuum laser absorption spectroscopy (SCLAS) are presented in order to quantify the conversion by detection of the produced H2O mole fraction. A single mode fiber (SMF) coupled setup is presented, with the fiber core acting as entrance slit of a Czerny-Turner spectrometer. Dependencies on residence time and global air-fuel ratio are presented at pressures up to 1.5 MPa and temperatures up to 900 K, at which distinct tracer and fuel consumption is observed. Signal loss due to intense beam steering was partially compensated using a self-stabilizing double-pass setup with a retroreflector.

X-ray Computed Tomography for Flame-Structure Analysis of Laminar Premixed Flames.

Quantitative X-ray computed tomography (XCT) diagnostics for reacting flows are developed and demonstrated in application to premixed flames in open and optically inaccessible geometries. A laboratory X-ray scanner is employed to investigate methane/air flames that were diluted with krypton as an inert radiodense tracer gas. Effects of acquisition rate and tracer gas concentration on the signal-to-noise ratio are examined. It is shown that statistically converged three-dimensional attenuation measurements can be obtained with limited impact from the tracer gas and within an acceptable acquisition time. Specific aspects of the tomographic reconstruction and the experimental procedure are examined, with particular emphasis on the quantification of experimental uncertainties. A method is developed to determine density and temperature from the X-ray attenuation measurements. These experiments are complemented by one- and multi-dimensional calculations to quantify the influence of krypton on the flame behavior. To demonstrate the merit of XCT for optically inaccessible flames, measurements of a complex flame geometry in a tubular confinement are performed. The use of a coflow to provide a uniform tracer-gas concentration is shown to improve the quantitative temperature evaluation. These measurements demonstrate the viability of XCT for flame-structure analysis and multi-dimensional temperature measurements using laboratory X-ray systems. Further opportunities for improving this diagnostic are discussed.

Time-Gated Single-Shot Picosecond Laser-Induced Breakdown Spectroscopy (ps-LIBS) for Equivalence-Ratio Measurements.

Time-gated picosecond laser-induced breakdown spectroscopy (ps-LIBS) for the determination of local equivalence ratios in atmospheric-pressure adiabatic methane-air flames is demonstrated. Traditional LIBS for equivalence-ratio measurements employ nanosecond (ns)-laser pulses, which generate excessive amounts of continuum, reducing measurement accuracy and precision. Shorter pulse durations reduce the continuum emission by limiting avalanche ionization. Furthermore, by contrast the use of femtosecond lasers, plasma emission using picosecond-laser excitation has a high signal-to-noise ratio (S/N), allowing single-shot measurements suitable for equivalence-ratio determination in turbulent reacting flows. We carried out an analysis of the dependence of the plasma emission ratio Hα (656 nm)/NII (568 nm) on laser energy and time-delay for optimization of S/N and minimization of measurement uncertainties in the equivalence ratios. Our finding shows that higher laser energy and shorter time delay reduces measurement uncertainty while maintaining high S/N. In addition to atmospheric-pressure flame studies, we also examine the stability of the ps-LIBS signal in a high-pressure nitrogen cell. The results indicate that the plasma emission and spatial position could be stable, shot-to-shot, at elevated pressure (up to 40 bar) using a lower excitation energy. Our work shows the potential of using ps-duration pulses to improve LIBS-based equivalence-ratio measurements, both in atmospheric and high-pressure combustion environments.

Combustion in the future: The importance of chemistry.

Combustion involves chemical reactions that are often highly exothermic. Combustion systems utilize the energy of chemical compounds released during this reactive process for transportation, to generate electric power, or to provide heat for various applications. Chemistry and combustion are interlinked in several ways. The outcome of a combustion process in terms of its energy and material balance, regarding the delivery of useful work as well as the generation of harmful emissions, depends sensitively on the molecular nature of the respective fuel. The design of efficient, low-emission combustion processes in compliance with air quality and climate goals suggests a closer inspection of the molecular properties and reactions of conventional, bio-derived, and synthetic fuels. Information about flammability, reaction intensity, and potentially hazardous combustion by-products is important also for safety considerations. Moreover, some of the compounds that serve as fuels can assume important roles in chemical energy storage and conversion. Combustion processes can furthermore be used to synthesize materials with attractive properties. A systematic understanding of the combustion behavior thus demands chemical knowledge. Desirable information includes properties of the thermodynamic states before and after the combustion reactions and relevant details about the dynamic processes that occur during the reactive transformations from the fuel and oxidizer to the products under the given boundary conditions. Combustion systems can be described, tailored, and improved by taking chemical knowledge into account. Combining theory, experiment, model development, simulation, and a systematic analysis of uncertainties enables qualitative or even quantitative predictions for many combustion situations of practical relevance. This article can highlight only a few of the numerous investigations on chemical processes for combustion and combustion-related science and applications, with a main focus on gas-phase reaction systems. It attempts to provide a snapshot of recent progress and a guide to exciting opportunities that drive such research beyond fossil combustion.

Data Processing Algorithm for Diagnostics of Combustion Using Diode Laser Absorption Spectrometry.

A new algorithm for the evaluation of the integral line intensity for inferring the correct value for the temperature of a hot zone in the diagnostic of combustion by absorption spectroscopy with diode lasers is proposed. The algorithm is based not on the fitting of the baseline (BL) but on the expansion of the experimental and simulated spectra in a series of orthogonal polynomials, subtracting of the first three components of the expansion from both the experimental and simulated spectra, and fitting the spectra thus modified. The algorithm is tested in the numerical experiment by the simulation of the absorption spectra using a spectroscopic database, the addition of white noise, and the parabolic BL. Such constructed absorption spectra are treated as experimental in further calculations. The theoretical absorption spectra were simulated with the parameters (temperature, total pressure, concentration of water vapor) close to the parameters used for simulation of the experimental data. Then, spectra were expanded in the series of orthogonal polynomials and first components were subtracted from both spectra. The value of the correct integral line intensities and hence the correct temperature evaluation were obtained by fitting of the thus modified experimental and simulated spectra. The dependence of the mean and standard deviation of the evaluation of the integral line intensity on the linewidth and the number of subtracted components (first two or three) were examined. The proposed algorithm provides a correct estimation of temperature with standard deviation better than 60 K (for T = 1000 K) for the line half-width up to 0.6 cm-1. The proposed algorithm allows for obtaining the parameters of a hot zone without the fitting of usually unknown BL.

All Fiber-Coupled OH Planar Laser-Induced-Fluorescence (OH-PLIF)-Based Two-Dimensional Thermometry.

Two-color, planar laser-induced fluorescence (PLIF)-based two-dimensional (2D) thermometry techniques for reacting flows, which are typically developed in the laboratory conditions, face a stiff challenge in their practical implementation in harsh environments such as combustion rigs. In addition to limited optical access, the critical experimental conditions (i.e., uncontrolled humidity, vibration, and large thermal gradients) often restrict sensitive laser system operation and cause difficulties maintaining beam-overlap. Thus, an all fiber-coupled, two-color OH-PLIF system has been developed, employing two long optical fibers allowing isolation of the laser and signal-collection systems. Two OH-excitation laser beams (∼283 nm and ∼286 nm) are delivered through a common 6 m long, 400 µm core, deep ultraviolet (UV)-enhanced multimode fiber. The fluorescence signal (∼310 nm) is collected by a 3 m long, UV-grade imaging fiber. Proof-of-principle temperature measurements are demonstrated in atmospheric pressure, near adiabatic, CH4/O2/N2 jet flames. The effects of the excitation pulse interval on fiber transmission are investigated. The proof-of-principle measurements show significant promise for thermometry in harsh environments such as gas turbine engine tests.

Applicability of Femtosecond Laser Electronic Excitation Tagging in Combustion Flow Field Velocity Measurements.

Femtosecond laser electronic excitation tagging (FLEET) is a molecular tagging velocimetry technique that can be applied in combustion flow fields, although detailed studies of its application in combustion are still needed. We report the applicability of FLEET in premixed CH4-air flames. We found that FLEET can be applied in all of the combustion areas (e.g., the unburned region, the burned region and the reaction zone). The FLEET signal in the unburned region is significantly higher than that in the burned region. This technique is suitable for both lean and rich CH4-air combustion flow fields and its performance in lean flames is better than that in rich flames.

Advanced Laser-Based Techniques for Gas-Phase Diagnostics in Combustion and Aerospace Engineering.

Gaining information of species, temperature, and velocity distributions in turbulent combustion and high-speed reactive flows is challenging, particularly for conducting measurements without influencing the experimental object itself. The use of optical and spectroscopic techniques, and in particular laser-based diagnostics, has shown outstanding abilities for performing non-intrusive in situ diagnostics. The development of instrumentation, such as robust lasers with high pulse energy, ultra-short pulse duration, and high repetition rate along with digitized cameras exhibiting high sensitivity, large dynamic range, and frame rates on the order of MHz, has opened up for temporally and spatially resolved volumetric measurements of extreme dynamics and complexities. The aim of this article is to present selected important laser-based techniques for gas-phase diagnostics focusing on their applications in combustion and aerospace engineering. Applicable laser-based techniques for investigations of turbulent flows and combustion such as planar laser-induced fluorescence, Raman and Rayleigh scattering, coherent anti-Stokes Raman scattering, laser-induced grating scattering, particle image velocimetry, laser Doppler anemometry, and tomographic imaging are reviewed and described with some background physics. In addition, demands on instrumentation are further discussed to give insight in the possibilities that are offered by laser flow diagnostics.

Laser-Induced Breakdown Spectroscopy (LIBS) for the Measurement of Spatial Structures and Fuel Distribution in Flames.

Laser-induced breakdown spectroscopy (LIBS) is used for the mapping of local structures (i.e., reactants and products zones) and for the determination of fuel distribution by means of the local equivalence ratio ϕ in laminar, premixed air-hydrocarbon flames. The determination of laser threshold energy to induce breakdown in the different zones of flames is employed for the identification and demarcation of the local structures of a premixed laminar flame, while complementary results about fuel concentration were obtained from measurements of the cyanogen (CN) band Β(2)Σ(+)--Χ(2)Σ(+), (Δυ = 0) at 388.3 nm and the ratio of the atomic lines of hydrogen (Hα) and oxygen (O(I)), Hα/O. The combination of these LIBS-based methods provides a relatively simple to use, rapid, and accurate tool for online and in situ combustion diagnostics, providing valuable information about the fuel distribution and the spatial variations of the local structures of a flame.

Direct Coherent Raman Temperature Imaging and Wideband Chemical Detection in a Hydrocarbon Flat Flame.

A single-shot coherent Raman imaging technique has been developed for spatially correlated one-dimensional high-fidelity gas-phase thermometry and multiplex chemical detection in flames. The technique utilizes two-beam phase matching, operating a single ultrashort pump/Stokes excitation pulse (7 fs) and a narrowband picosecond probe pulse (70 ps), interrogating a Raman active window of ∼4200 cm(-1) with ∼0.3 cm(-1) spectral resolution. The measurement geometry is formed intersecting the two beams shaped as laser-sheets and the one-coordinate spatial information is retrieved with a linespread function of <40 µm. The advance provides the possibility for the multiplexed measurement of all combustion relevant major species simultaneously with gaseous temperature monitored over a several millimeter field of view. The current technique is optimized in a premixed hydrocarbon flat-flame. At the flame-front, it is shown that direct imaging renders the temperature profile within ∼1% inaccuracy, whereas typical point-wise raster scanning may have relative systematic deviations up to 15% due to spatial averaging effects.

Diagnostic Imaging in Flames with Instantaneous Planar Coherent Raman Spectroscopy.

Spatial mapping of temperature and molecular species concentrations is vitally important in studies of gaseous chemically reacting flows. Temperature marks the evolution of heat release and energy transfer, while species concentration gradients provide critical information on mixing and chemical reaction. Coherent anti-Stokes Raman spectroscopy (CARS) was pioneered in measurements of such processes almost 40 years ago and is authoritative in terms of the accuracy and precision it may provide. While a reacting flow is fully characterized in three-dimensional space, a limitation of CARS has been its applicability as a point-wise measurement technique, motivating advancement toward CARS imaging, and attempts have been made considering one-dimensional probing. Here, we report development of two-dimensional CARS, with the first diagnostics of a planar field in a combusting flow within a single laser pulse, resulting in measured isotherms ranging from 450 K up to typical hydrocarbon flame temperatures of about 2000 K with chemical mapping of O2 and N2.