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Nous avons mis en place un dispositif permettant l’acquisition d'échos de photons stimulés infrarouges à l’échelle femtoseconde. Le but est d'examiner la dynamique vibrationnelle aux temps courts de métaux carbonyles (W(CO)₆ and Fe(CO)₅) piégés en matrice cryogénique (4-50 K). Cet environnement solide, issu de la condensation d'un mélange gazeux contenant une impureté et un gaz inerte (N₂, CH₄, Ar, etc.), est propice à l’étude de systèmes dans leur état fondamental. L’excitation d’une vibration moléculaire s’atténue toujours temporellement, ce qui correspond dans le domaine spectral à un élargissement des raies d’absorption. L’étude de la dynamique vibrationnelle vise à examiner les causes physiques à l’origine de cet élargissement spectral. Typiquement, elles sont de trois sortes : phénomènes intramoléculaires, interactions entre molécules piégées et interactions entre la molécule piégée et l’environnement. Les échos de photons permettent de distinguer les contributions homogènes et inhomogènes de l’élargissement spectral et de caractériser les processus de déphasage, de relaxation des populations et de diffusion spectrale. Parmi les résultats obtenus, nous avons mis en évidence l'influence des phonons spécifiques aux matrices moléculaires (ex : libration de N₂ et rotation de CH₄ ) sur le déphasage vibrationnel ainsi que l’influence de la transition de phase du méthane solide à 20 K sur la dynamique vibrationnelle. Nous avons également montré que la dynamique vibrationnelle était dépendante du site cristallographique dans lequel est piégée la molécule. Enfin, en excitant plusieurs modes de vibration simultanément, nous avons pu examiner les couplages intramoléculaires. / We built an experimental set-up in order to generate infrared stimulated photon echoes at the femtosecond timescale. The purpose is to examine the short time vibrational dynamics of metal carbonyls (W(CO)₆ and Fe(CO)₅) trapped in cryogenic matrices (4-50 K). This environment, resulting from the condensation of a gas mixture containing the impurity and an inert gas (N₂, CH₄, Ar, etc.), is well suited to study systems in their ground state. An excited molecular vibration is always damped in the time domain. It corresponds in the frequency domain to a broadening of the absorption line. The study of the vibrational dynamics aims at examining the physical causes of this spectral broadening. Typically, there are three kinds of causes: intramolecular phenomena, interactions between trapped molecules and interactions between the impurity and the environment. Photon echoes allow distinguishing between the homogeneous and the inhomogeneous contributions of the spectral broadening and characterizing dephasing process, population relaxation and spectral diffusion. Among the obtained results, we highlighted the influence of phonons that are specific to molecular matrices (ex: N₂ libration and CH₄ rotation) on the vibrational dephasing. Moreover, we observed the influence of the phase transition of solid methane at 20 K on the vibrational dynamics. We also showed that the vibrational dynamics depends on the site in which the molecule is trapped. Finally, when exciting several vibrational modes, we are also able to study intramolecular couplings.

The hypersonic laminar to turbulent transition problem above Mach 10 is addressed experimentally in the short duration VKI Longshot gun tunnel. Reentry conditions are partially duplicated in terms of Mach and Reynolds numbers. Pure nitrogen is used as a test gas with flow enthalpies sufficiently low to avoid its dissociation, thus approaching a perfect gas behavior. The stabilizing effects of Mach number and nosetip bluntness on the development of natural boundary layer disturbances are evaluated over a 7 degrees half-angle conical geometry without angle of attack. <p><p>Emphasis is initially placed on the flow characterization of the Longshot wind tunnel where these experiments are performed. Free-stream static pressure diagnostics are implemented in order to complete existing stagnation point pressure and heat flux measurements on a hemispherical probe. An alternative method used to determine accurate free-stream flow conditions is then derived following a rigorous theoretical approach coupled to the VKI Mutation thermo-chemical library. Resulting sensitivities of free-stream quantities to the experimental inputs are determined and the corresponding uncertainties are quantified and discussed. The benefits of this different approach are underlined, revealing the severe weaknesses of traditional methods based on the measurement of reservoir conditions and the following assumptions of an isentropic and adiabatic flow through the nozzle. The operational map of the Longshot wind tunnel is redefined accordingly. The practical limits associated with the onset of nitrogen flow condensation under non-equilibrium conditions are also accounted for. <p><p>Boundary layer transition experiments are then performed in this environment with free-stream Mach numbers ranging between 10-12. Instrumentation along the 800mm long conical model includes flush-mounted thermocouples and fast-response pressure sensors. Transition locations on sharp cones compare favorably with engineering correlations. A strong stabilizing effect of nosetip bluntness is reported and no transition reversal regime is observed for Re_RN<120000. Wavelet analysis of wall pressure traces denote the presence of inviscid instabilities belonging to Mack's second mode. An excellent agreement with Linear Stability Theory results is obtained from which the N-factor of the Longshot wind tunnel in these conditions is inferred. A novel Schlieren technique using a short duration laser light source is developed, allowing for high-quality flow visualization of the boundary layer disturbances. Comparisons of these measurement techniques between each other are finally reported, providing a detailed view of the transition process above Mach 10. / Doctorat en Sciences de l'ingénieur / info:eu-repo/semantics/nonPublished