Les progrès technologiques des dispositifs expérimentaux ainsi que les récentes avancées pour la simulation des spectres Raman à haute température rendent aujourd’hui possible la mise en oeuvre d’une technique de mesures multi-espèces de température et de concentration uniquement fondée sur l’ajustement des spectres mono-coups de diffusion Raman spontanée collectés au sein des flammes turbulentes. Dans cette étude, cette stratégie de post-traitement, associée à une chaîne de mesure spécifique, est développée selon plusieurs axes pour permettre l’extension des mesures à des cas de flammes ordinairement hostiles aux mesures classiques Rayleigh/Raman résolues par inversion matricielle ou par méthode hybride. Dans une flamme diphasique d’éthanol, une thermométrie fondée sur l’ajustement des spectres de N2 a été mise en place afin de s’affranchir des contraintes liées à la diffusion de Mie des gouttes. L’intégration d’une thermométrie Raman à partir du spectre du méthane ainsi que d’une procédure de minimisation de l’émission de C2 dans le post-traitement des spectres ont permis la réalisation de cartographies multi-scalaires (température et toutes espèces majoritaires) dans toute la zone de recirculation d’une flamme turbulente légèrement fuligineuse générée par un brûleur bluff-body. Une thermométrie fondée sur la minimisation du spectre Raman de CO2 a également été développée et éprouvée au cours d’une campagne de mesures dans une installation d’échelle semi-industrielle reproduisant les conditions d’oxycombustion des cycles de turbines à gaz dans l’objectif de la capture et de la séquestration du CO2. / Recent progress in experimental devices and simulation of high-temperature Raman spectra enable the implementation of a spectral fitting method to solve single-shot Spontaneous Raman Scattering spectra collected in turbulent flames. In this study, this post-processing method, associated to a specific experimental set-up, has been developed to extend measurements to several cases of non-Raman friendly flames where matrix inversion or hybrid methods are usually limited. In a two-phase flame, N2 Raman thermometry has been used to overcome issues from Mie scattering of droplets. The implementation of a CH4 Raman thermometry and a minimization procedure of C2 emission in the data post-processing allowed the achievement of multi-scalar cartographies (temperature and all major species) throughout the recirculation zone of a slightly sooting turbulent flame stabilized on a bluff-body burner. A thermometry based on the minimization of CO2 Raman spectrum has also been developed and tested during a measurement campaign in a semi-industrial scale installation designed for the study of oxyfuel gas turbine cycle in the aim of carbon capture and sequestration.

<p>Ultrafast laser-based diagnostic techniques are powerful tools for the detailed understanding of highly dynamic combustion chemistry and physics. The ultrashort pulses provide unprecedented temporal resolution along with high peak power for broad spectral range−ideal for nonlinear signal generation at high repetition rate−with applications including next-generation combustors for gas turbines, plasma-assisted combustion, hypersonic flows and rotating detonation engines. The current work focuses on advancing (i) femtosecond (fs) two-photon laser-induced fluorescence, and (ii) hybrid femtosecond/picosecond vibrational and rotational coherent anti-Stokes Raman scattering (fs/ps RCARS and VCARS) to higher pressures for the first time. </p><p>Quantitative single-laser-shot kHz-rate concentration measurements of key atomic (O-atom) and molecular (CO) species is presented using femtosecond two-photon laser-induced fluorescence (TP-LIF) for a range of equivalence ratios and pressures in diffusion flames. A multitude of signal-interfering sources and loss mechanisms−relevant to high-pressure fs TP-LIF applications−are also quantified up to 20 atm to ensure high accuracy. The pressure scaling of interferences take into account degradation, attenuation and wave-front distortion of the excitation laser pulse; collisional quenching and pressure dependent transition line-broadening and shifting; photolytic interferences; multi-photon ionization; stimulated emission; and radiation trapping. </p><p>Hybrid fs/ps VCARS of N₂ is reported for interference-free temperature measurement at 1300-2300 K in high-pressure, laminar diffusion flames up to 10 atm. A time asymmetric probe pulse allowed for detection of spectrally resolved CARS signals at probe delays as early as ~200-300 fs while being independent of collisions for the full range of pressures and temperatures. Limits of collisional independence, accuracy and precision of the measurement is explored at various probe-pulse delays, pressures and temperatures. </p><p> </p><p>Additionally, a novel all diode-pumped Nd:YAG amplifier design is presented for generation of time-synchronized ps-probe pulses for hybrid fs/ps RCARS of N₂. High-energy, nearly transform-limited, single-mode, chirp-free ps probe-pulses are generated at variable pulsewidths. The detailed architecture and characterization of the laser is presented. kHz-rate RCARS thermometry is presented up to 2400 K. Excellent spatial, spectral, and temporal beam quality allowed for fitting the theoretical spectra with a simple Gaussian model for the probe pulse with temperature accuracies of 1-2%. </p> <p><br></p>