CARS temperature measurement in a LOX/CH4 spray flame

Coherent anti‐Stokes Raman scattering (CARS) spectroscopy has been used to investigate cryogenic liquid oxygen/gaseous methane (LOX/CH₄) flames on a medium‐size test facility at a pressure of 0.24 MPa and mass flow of 0.025 kg/s. Single‐shot, broadband CARS spectra with simultaneous detection of the Q‐branches of hydrogen and water molecules were recorded with good signal‐to‐noise ratio. Temperature was deduced from the H₂ and H₂O CARS profiles. The spatial temperature distribution in a comparatively harsh environment has been measured successfully. The measurements took place in the windowed combustion chamber of the DLR M3 test facility, aiming to provide data for validation of rocket combustor modeling. Copyright © 2010 John Wiley & Sons, Ltd.     

Single‐shot CARS thermometry of high‐pressure hydrocarbon flames using simultaneous intensity and linewidth measurements

We demonstrate the feasibility of single laser shot coherent anti‐Stokes Raman scattering thermometry with simultaneous measurement of intensities of hydrogen Q‐branch lines and their linewidths in a pulsed CH₄/O₂ combustion chamber operating at 20 MPa pressure and 3000 K temperature—parameters that are typical for full‐scale rocket engines. The measurements were done by means of a spectrograph combined with an interferometer having orthogonal directions of dispersions. This approach allows correct temperature evaluation that takes into account the directly measured linewidths. Copyright © 2010 John Wiley & Sons, Ltd.     

Random lasing in an organic light‐emitting crystal and its interplay with vertical cavity feedback

The simultaneous vertical‐cavity and random lasing emission properties of a blue‐emitting molecular crystal are investigated. The 1,1,4,4‐tetraphenyl‐1,3‐butadiene samples, grown by physical vapour transport, feature room‐temperature stimulated emission peaked at about 430 nm. Fabry‐Pérot and random resonances are primed by the interfaces of the crystal with external media and by defect scatterers, respectively. The analysis of the resulting lasing spectra evidences the existence of narrow peaks due to both the built‐in vertical Fabry‐Pérot cavity and random lasing in a novel, surface‐emitting configuration and threshold around 500 μJ cm⁻². The anti‐correlation between different modes is also highlighted, due to competition for gain. Molecular crystals with optical gain candidate as promising photonic media inherently supporting multiple lasing mechanisms.     

High temperature O2-CARS thermometry

O₂ temperature measurements at T=1910K have been performed by coherent anti-Stokes Raman scattering (CARS) inside a homogeneously heated gas volume of a tube furnace. The oxygen CARS spectrum can now be modeled accurately within the higher vibrational levels of the Q-branch manifold populated at flame temperatures using recently available spectroscopic data and collisional broadening coefficients.     

Rotational CARS N2 thermometry: validation experiments for the influence of nitrogen spectral line broadening by hydrogen

Rotational coherent anti‐Stokes Raman spectroscopy (CARS) in fuel‐rich hydrocarbon flames, with a large content of hydrogen in the product gases (∼20%), has in previous work shown that evaluated temperatures are raised several tens of Kelvin by taking newly derived N₂ H₂ Raman line widths into account. To validate these results, in this work calibrated temperature measurements at around 300, 500 and 700 K were performed in a cell with binary gas mixtures of nitrogen and hydrogen. The temperature evaluation was made with respect to Raman line widths either from self‐broadened nitrogen only, N₂ N₂ [energy‐corrected‐sudden (ECS)], or by also taking nitrogen broadened by hydrogen, N₂ H₂ [Robert–Bonamy (RB)], Raman line widths into account. With increased amount of hydrogen in the cell at constant temperature, the evaluated CARS temperatures were clearly lowered with the use of Raman line widths from self‐broadened nitrogen only, and the case with inclusion of N₂ H₂ Raman line widths was more successful. The difference in evaluated temperatures between the two different sets increases approximately linearly, reaching 20 K (at T ∼ 300 K), 43 K (at T = 500 K) and 61 K (at T = 700 K) at the highest hydrogen concentration (90%). The results from this work further emphasize the importance of using adequate Raman line widths for accurate rotational CARS thermometry. Copyright © 2010 John Wiley & Sons, Ltd.     

The application of CARS for temperature measurements in high pressure combustion systems

The determination of accurate temperatures from CARS N₂ Q-branch spectra in premixed flames is discussed for pressures up to 40 bar. The influence of collisional line narrowing in the CARS spectra is modelled by a MEG fitting law. It takes into account collisions of N₂ with CO₂ and H₂O. The analysis of the CARS data showed that the non-resonant background has an increasing influence on temperature with increasing pressure. Little influence on the quality of the fit between theory and experiment was found. Since there is a danger of residual systematic temperature deviations, which cannot be identified from the quality of the fit, spontaneous rotational Raman scattering is employed as an independent measuring technique.     

Semiclassical line broadening calculations,using an ab initio potential energy surface,in Q‐branch and S‐branch of N2 perturbed by H2

In order to improve the accuracy of Raman combustion diagnostics, the broadening coefficients of N₂ perturbed by H₂ for Q‐branch and S‐branch have been calculated by the semiclassical Robert–Bonamy model using an ab initio potential energy surface. The calculations have been performed for a large range of temperatures (from 77 to 800 K) and J rotational quantum numbers (from 0 to 60). This paper shows that our results and their temperature dependence are in good agreement with earlier published experimental and theoretical data. Moreover, our results improve the semiclassical calculations made earlier with an adapted analytical potential. The results, obtained at high temperatures and for a large range of rotational quantum numbers, are presented in order to be implemented for optical diagnostics in combustion media. Copyright © 2012 John Wiley & Sons, Ltd.     

H2 CARS thermometry in a fuel-rich,premixed, laminar CH4/air flame in the pressure range between 5 and 40 bar

To establish H₂ CARS thermometry at high pressure, accumulated H₂ Q-branch CARS spectra were recorded in the exhaust of a fuel-rich CH₄/air flame at pressures between 5 and 40 bar. Temperatures were deduced by fitting theoretical spectra to experimental data points. The Energy-Corrected Sudden (ECS) scaling law was employed to set up an empirical model for the calculation of H₂ linewidths in high-pressure hydrocarbon flames with H₂ as a minority species. Experimental H₂ CARS spectra could be simulated very accurately with this model. The evaluated temperatures agreed well with reference temperatures obtained by spontaneous rotational Raman scattering of N₂.     

A single mode flashlamp-pumped dye laser

A flashlamp-pumped dye laser capable of single transverse and longitudinal mode operation is described. The maximum untuned power output is 2 MW cm^-2, TEM₀₀ mode. By employing three intracavity Fabry—Pérot etalons, a minimum spectral width of 4 MHz, stable to within 12 MHz, has been obtained.     

Experimental natural lifetime determination of the Ar(II) lower laser levels

The natural lifetimes of the (³P)4s²P_3/2,1/2 levels of the Ar(II) spectrum have been determined from the natural broadening of argon lines, measured with a Fabry—Pérot interferometer. The natural broadening was determined from the lines with wavelengths of 4880 and 4965 Å by comparing them with the lines at 4806 and 5009 Å having negligible natural broadening. The natural lifetime of the 4s²P_3/2 level appeared to be τ = 0.19 (±6%) ns and of the 4s²P_1/2 level τ = 0.18 (±15%) ns. These values are about 1.5 to 2 times as small as those determined by other authors either experimentally by using a Fabry—Pérot interferometer by the method of Ballik, or calculated using intermediate coupling.The differences between the two experimental methods are discussed.     

Backscattering mirrors for X-rays and Mössbauer radiation

Observation of exact backscattering of X-rays and studies of its energy and angular dependences; test of the validity of the dynamical theory of diffraction in the extreme case of exact backscattering; backscattering high-energy-resolution monochromators; backscattering interferometers, in particular of the Fabry–Pérot interferometer type; and precise, up to 5·10^—9 Å, measurements of crystal lattice parameters: these are central topics of the paper. Special attention is paid to the selection of crystals to be used as backscattering mirrors. Noncubic crystals like Al₂O₃, SiC, etc., allow backscattering for X-rays with practically any energy above 10 keV. Feasibility of backscattering mirrors for Mössbauer radiation of ⁵⁷Fe (14.4 keV), ¹⁵¹Eu (21.5 keV), ¹¹⁹Sn (23.9 keV), and ¹⁶¹Dy (25.6 keV) nuclei is demonstrated by Al₂O₃ crystals. A concrete design of a sapphire Fabry–Pérot–Bragg étalon is presented.

     

Study of processes of translational,rotational, and vibrational relaxation based on CARS spectra line shapes

This paper reviews the various physico-chemical processes responsible for actual linewidths encountered in high-resolution coherent anti-Stokes Raman spectroscopy (CARS). Most of the experimental data are based on linewidth measurements using a pulseamplified CARS spectrometer with an emission bandwidth (FWHM) of 2×10^–3 cm^–1. Detailed rotational and vibrational relaxation constants have been obtained from the analysis of theQ-branch profiles of C₂H₂, N₂, CH₄, and SiH₄.     

Optical diagnostic of temperature in rocket engines by coherent Raman techniques

This article reviews the study of Raman line shapes of molecular species involved in reactive media, such flames or engines, at high temperature and high pressure. This study is of interest from a fundamental as well as from a practical point of view with regards to the CARS temperature diagnostic of GH₂–LOX combustion systems. We will particularly draw attention to recent investigations by means of Stimulated Raman Spectroscopy (SRS) in H₂–H₂O mixtures at temperature up to 1800 K. Whereas H₂–X systems usually exhibit large inhomogeneous effects, due to the speed dependence of the collisional parameters, the absence of such apparent inhomogeneous signatures in the H₂–H₂O system allowed us to model the broadening coefficients with simple polynomial laws. These laws permit extrapolations with a narrow confidence interval, as required for temperature measurements. The applications of these results to the temperature diagnostic on the small-scale facility MASCOTTE at ONERA will be described. To cite this article: F. Chaussard et al., C. R. Physique 5 (2004).     

Polarization‐sensitive CARS spectroscopy on free‐base porphyrins: coproporphyrin I tetramethyl ester

The application of polarization‐sensitive (PS) coherent anti‐Stokes Raman scattering (CARS) spectroscopy for the investigation of highly luminescent free‐base porphyrins under Q_x band resonance is discussed. For coproporphyrin I tetramethyl ester (CP‐I‐TME), PS CARS spectra involving resonances with the electronic Q_x absorption band as well as polarized spontaneous Raman spectra involving B band resonance are presented. A quantitative evaluation of the CP‐I‐TME spectra is performed and the results are compared to our previously presented data on free‐base octaethylporphine (OEP) and mesoporphyrin IX dimethyl ester (MP‐IX‐DME), which were obtained under identical excitation conditions. This comprehensive analysis reveals several spectral differences that can be attributed to the different β–substitution pattern of the porphyrin macrocycle. Additionally, the strong resonance enhancement of totally symmetric modes under Q_x band excitation is identified as a common property for OEP, CP‐I‐TME, and MP‐IX‐DME; this enhancement selectivity distinguishes the investigated substances from what is generally observed for metallo porphyrins. Copyright © 2008 John Wiley & Sons, Ltd.     

Dual-pump coherent anti-Stokes Raman scattering thermometry in a sooting turbulent pool fire

We present a dual-pump coherent anti-Stokes Raman scattering (CARS) instrument, which has been constructed for the probing of temperature fluctuations in turbulent pool fires of meter-scale. The measurements were performed at the Fire Laboratory for Accreditation of Models and Experiments (FLAME) facility at Sandia National Laboratories, which provides a canonical fire plume in quiescent wind conditions, with well-characterized boundary conditions and access for modern laser-diagnostic probes. The details of the dual-pump CARS experimental facility for the fire-science application are presented, and single-laser-shot CARS spectra containing information from in-fire N₂, O₂, H₂, and CO₂ are provided. Single-shot temperatures are obtained from spectral fitting of the Raman Q-branch signature of N₂, from which histograms that estimate the pdf of the enthalpy-averaged temperature fluctuations at the center of the fire plume are presented. Results from two different sooting fire experiments reveal excellent test-to-test repeatability of the fire plume provided by FLAME, as well as the CARS-measured temperatures. The accuracy and precision of the CARS temperatures is assessed from measurements in furnace-heated air, where the temperature can be accurately determined by a thermocouple. At temperatures in excess of 500 K, the furnace results show that the CARS measurements are accurate to within 2-3% and precise to within ±3-5% of the measured absolute temperature.     

H2 vibrational spectral signatures in binary and ternary mixtures: theoretical model,simulation and application to CARS thermometry in high pressure flames

A summary of the main results obtained by the two groups in the field of H₂ vibrational spectral line signatures for various mixtures, in connection with CARS diagnostics of H₂–O₂ combustion systems, is presented. H₂–X systems may have specific large inhomogeneous spectral features, due to the dependence of the line broadening and line shifting on the (H₂) radiator speed, particularly at high temperature. Thus, careful attention has to be paid to rigorously analyze such features, both from the experimental point of view (Dijon) and from the theoretical one (Besançon). Applications of the present results to high-pressure H₂/air flame thermometry are also briefly described. They present an approach aiming to include the more recent basic results on coherent Raman line shape in CARS diagnostics, in order to improve the accuracy of temperature measurements.     

High-Sensitivity Temperature Sensor Based on Two Parallel Fabry–Pérot Interferometers and Vernier Effect

Journal of Russian Laser Research - We propose a novel sensor with its temperature sensitivity improved by the Vernier effect. The sensor comprises two parallel Fabry–Pérot...     

Hydrogen CARS thermometry in a high-pressure H2–air flame. Test of H2 temperature accuracy and influence of line width by comparison with N2 CARS as reference

This work describes a further step towards the determination of the temperature accuracy of H₂ Q-branch CARS (Coherent Anti-Stokes Raman Scattering) at high pressure with regard to the influence of the H₂ line widths. In laminar steady H₂/air flames in the pressure range 1–15 bar and at fuel-rich conditions with stoichiometries between two and four, quasi-simultaneous temperature measurements were performed with H₂ and N₂ CARS. The temperature values deduced from H₂ CARS are in good agreement with the reference temperature from N₂ CARS. The influence of different line-width contributions on the accuracy of H₂ Q-branch thermometry was investigated in detail. Received: 10 April 2001 / Revised version: 22 May 2001 / Published online: 18 July 2001     

Laser-induced fluorescence determination of flame temperatures in comparison with CARS measurements

Temperature profiles in several premixed low pressure H₂/O₂/N₂ flames and in an atmospheric pressure CH₄/air flame were determined by laser-induced fluorescence (LIF) and by CARS experiments. In the LIF study, temperatures were derived from OH excitation spectra, CARS temperatures were deduced from N₂ Q-branch spectra. The present study is the first quantitative comparison of these two methods for temperature determination in flames burning at pressures up to 1 bar. The resulting temperatures showed good agreement.     

Time‐resolved investigation of the ν1 ro‐vibrational Raman band of H2CO with fs‐CARS

The technique of femtosecond time‐resolved coherent anti‐Stokes scattering (fs‐CARS) is used to investigate the strongly perturbed ν₁ ro‐vibrational Raman band of formaldehyde (H₂CO). The time‐dependent signal is simulated using a ‘Watson‐’Hamiltonian in A‐type reduction and Raman theory for asymmetric rotors. The results are compared with the experimental data. The fs‐CARS method measures the evolution of the polarization in a molecular ensemble via superposition of many states and is sensitive to spectral irregularities or line shifts of the involved transitions. ‘Coriolis’ interactions play a major role in the analysis of the ν₁ band of formaldehyde. We successfully simulate the fs‐CARS transient signal from the ν₁ band of formaldehyde including a model for multiple ‘Coriolis’ interactions, without the necessity of describing the complete interaction between all the vibrational levels. ‘Coriolis’ coupling coefficients and energy shifts are derived from the experiment by a least‐square fit. The results are discussed and compared to literature values. Copyright © 2006 John Wiley & Sons, Ltd.