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International audience; We present a simple approach to predict the main features of optical spectra affected by self-phase modulation (SPM), which is based on regarding the spectrum modification as an interference effect. A two-wave interference model is found sufficient to describe the SPM-broadened spectra of initially transform-limited or up-chirped pulses, whereas a third wave should be included in the model for initially down-chirped pulses. Simple analytical formulae are derived, which accurately predict the positions of the outermost peaks of the spectra.

International audience; We discuss the effects of imparting a temporal sinusoidal phase modulation to a continuous wave on the frequency spectrum. While a practical analytical solution to this problem already exists, we present here a physical interpretation based on interference processes. This simple model will help the students better understand the origin of the oscillatory structure that can be observed in the resulting spectrum and that is characteristic of Bessel functions of the first kind. We illustrate our approach with an example from the field of optics.

International audience; We theoretically study the effects of the temporal intensity profile of the initial pulse on the nonlinear spectral compression process arising from nonlinear propagation in an optical fibre. Various linearly chirped input pulse profiles are considered, and their dynamics is explained with the aid of time-frequency representations. While initially parabolic-shaped pulses show enhanced spectral compression compared to Gaussian pulses, no significant spectral narrowing occurs when initially super-Gaussian pulses are used. Triangular pulses lead to a spectral interference phenomenon similar to the Fresnel bi-prism experiment.

International audience; Experimental and theoretical investigations of coherent anti-Stokes Raman spectroscopy of CH4 have been carried out. Experimental spectra were measured in a heated high-pressure test cell and compared with numerical simulations. Good agreement was obtained for the temperature and the pressure dependence of CARS spectra in the ranges 300-1100 K and 0.1-5.0 MPa. The observed dependencies provide useful guidance for CARS thermometry, allowing quantitative measurements of temperature in high-pressure combustors. Application of multiplex CH4 CARS thermometry for single-shot measurements in a LOX/CH4 combustion at high pressure was demonstrated at supercritical conditions (5.6 MPa).

International audience; The dynamics of the ferric CN complexes of the heme proteins Myoglobin and Hemoglobin I from the clam Lucina pectinata upon Soret band excitation is monitored using infrared and broad band visible pump-probe spectroscopy. The transient response in the UV-vis spectral region does not depend on the heme pocket environment and is very similar to that known for ferrous proteins. The main feature is an instantaneous, broad, short-lived absorption signal that develops into a narrower red-shifted Soret band. Significant transient absorption is also observed in the 360 - 390 nm range. At all probe wavelengths the signal decays to zero with a longest time constant of 3.6 ps. The infrared data on MbCN reveal a bleaching of the C = N stretch vibration of the heme-bound ligand, and the formation of a five-times weaker transient absorption band, 28 cm(-1) lower in energy, within the time resolution of the experiment. The MbC = N stretch vibration provides a direct measure for the return of population to the ligated electronic ( and vibrational) ground state with a 3 - 4 ps time constant. In addition, the CN-stretch frequency is sensitive to the excitation of low frequency heme modes, and yields independent information about vibrational cooling, which occurs on the same timescale.

International audience; Time-resolved detection of field-free molec- ular alignment is investigated by phase contrast. The technique based on a 4f imager operating as an inverted Zernike spatial filter makes it possible to discriminate be- tween positive and negative molecular alignment revivals produced in a linear molecule. The measurements are performed in a way that minimizes the contamination of the signal by the plasma generated during the align- ing pulse. The observations are supported by a semi- analytical model, from which the degree of alignment produced at the beam focus is estimated.

International audience; CARS laboratory experiments were done in the 2905-2925 cm(-1) range, in the vicinity of the v, band of the methane molecule, for pressures ranging from I to 50 bar, and temperatures up to 1100 K. These experiments were carried out in order to retrieve the pressure evolution of the CH4 spectrum, as well as to confirm its temperature dependance. After a brief recall on the theory used to compute pressure broadening coefficients and relaxation rates, we consider the v(3) and v(4) infrared bands of methane for benchmark calculations purposes. Next, we present recent experimental CARS spectra and calculated ones. Lastly, we discuss flame experiments as well as comparisons of temperature retrieval using N-2 and CH4 as probe molecules.

International audience; We present a study of the spontaneous Raman spectra of (CH4)-C-12 from 1200 to 5500 cm(-1) at various temperatures. This study is of interest from a fundamental as well as from a practical point of view with regards to the temperature diagnostic in hydrocarbon combustion. The present investigation shows that the spontaneous (CH4)-C-12 Raman spectra are very sensitive to temperature and that the complexity of methane spectra is not an obstacle to use methane as a probe molecule in laser-diagnostic techniques. Our study consists in determining the polarisability parameters of methane (CH4)-C-12, unknown at the present time, from spontaneous Raman spectra recorded at pressure less than one atmosphere to minimize the problem of line-mixing. This diagnostic method technique based on spontaneous Raman spectroscopy may be applied to temperature measurements in a uni-element rocket combustion chamber using methane-oxygen propellants.

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).

International audience; Rotational coherent anti-Stokes Raman spectroscopy (CARS) is a well-established spectroscopic technique for thermometry at pre-combustion temperatures an atmospheric pressure. However, at pressures of several MPa, a previous investigation revealed large discrepancies between experimental data and the theoretical model. A re-evaluation has been made of these data (at room temperature and in the range 1.5-9 MPa) with two improvements to the spectral code. The first is the inclusion of an inter-branch interference effect, which is described in detail in Paper I. The second is the use of experimental S-1-branch Raman line widths measured at 295 K, with a temperature dependence extracted from semi-classical calculations following the Robert-Bonamy formalism. It is shown that these two modifications significantly improve the theoretical model, since both the spectral fits and the accuracy of the evaluated temperatures are considerably improved.

International audience; In the present paper, we investigate the saturation mechanism of FDFWM (forward degenerate four-wave-mixing) spectra, observed with different polarizations of the input beams, line coupling, and Doppler effect. Our theoretical approach uses a nonperturbative resolution of the density matrix equations, decomposed on the irreducible tensor basis. This formalism greatly simplifies analytical expressions and allows for a correct treatment of magnetic sublevels structure in a three-J level system. Systematic calculations of the FDFWM signal for specific NO lines are performed to characterize intensities and line shapes as a function of saturation. Relative intensities exhibit strong changes in the intermediate regime of saturation further supporting the necessity for using such a complete model. Under saturating conditions, line coupling is shown to distort the spectra, according to the type of transition and the polarization configuration. This effect is observed in the following paper [V. Kruger et al., paper II, Phys. Rev. A 64, 012717 (2001)], where saturated experimental spectra of NO are presented and interpreted for two polarization configurations of interest for diagnostic purposes.

In this paper, we present measurements and modeling of femtosecond time resolved coherent anti-Stokes Raman spectroscopy (CARS) signal in H(2)-N(2) mixtures at low densities. Three approaches have been used to model the CARS response. The first is the usual sum of Voigt profiles. In the second approach, the speed dependent Voigt profile is used. In the last approach, a model of the temporal CARS signal is developed, which takes into account the velocity changes induced by collisions and the speed dependence of the collisional parameters. The velocity changes are modeled using the Keilson and Storer memory function; the radiator speed dependences of the collisional parameters are determined from their temperature dependences. The results obtained are consistent with previous studies in the frequency domain, showing that the changes of the velocity have important effects for the H(2)/N(2) system in the Dicke narrowing density regime.

This thesis is devoted to the study of dynamics induced by intense femtoseconds lasers pulses. The first studied dynamics deals with molecular alignment of CO2-X mixtures (X=CO2, Ar, N2), in dense gases (up to 20 bar). Up to now, this regime has never been studied experimentally. In the field-free regime (after laser/matter interaction), molecular alignment exhibits two components : a permanent alignment and a transient one. The influence of collisions appears through population transfers between rotational states, which leads to a decrease of these two contributions. Permanent alignment relaxation time is only tied to inelastics collisions whereas transient alignment relaxation time is tied to both inelastics and elastics ones. We show that the determination of the elastic collisions contribution (for which the experimental determination is uneasy), is then possible thanks to the analysis of molecular alignment measurements. This analysis is based on the modelling of inelastics rotational state-to-state transfer rates by ECS-(E)P semi-empirical laws. The elastic contribution of collisions is experimentally determined and happened to be in a good agreement with classically calculated ones. The second studied dynamics is the intensity dependence of the electronic Kerr effect. We pursue the works led by Loriot and al. in 2009 which showed that electronic Kerr index saturated, before nullifying and then presenting a negative contribution when the intensity increases (inversion of the sign for some tens of terawatts by square centimeter). We complete the previous study by performing similar measurements in air at 400 nm (800 nm in the original study)., Le sujet de cette thèse concerne l’étude de dynamiques induites par des impulsions lasers femtosecondes intenses. La première dynamique étudiée porte sur l’alignement de la molécule de CO2, pure ou en mélange avec l’argon ou l’hélium, en phase gazeuse dense (jusqu’à 20 bar), ce régime n’ayant jamais été étudié expérimentalement auparavant. L’alignement moléculaire, quand il est induit par une impulsion laser femtoseconde et intense, présente deux contributions qui apparaissent après passage de l’impulsion : un alignement permanent et un alignement transitoire. L’influence des collisions se manifeste alors par des transferts de population entre états rotationnels qui ont pour conséquence de faire décroître ces deux contributions. Le temps de décroissance de l’alignement permanent est seulement lié aux collisions inélastiques tandis que le temps de décroissance de l’alignement transitoire est lié à la fois aux collisions inélastiques et élastiques. Nous montrons alors que la détermination expérimentale de la contribution des collisions élastiques, expérimentalement difficile d’accès, est possible à partir de l’analyse des traces d’alignement moléculaire. Cette analyse se base sur la modélisation des taux de transfert entre états liés aux collisions inélastiques par des lois semi-empiriques du type ECS-(E)P. La contribution élastique des collisions déterminée est en bon accord avec des valeurs calculées selon un modèle classique. La deuxième dynamique étudiée est la dépendance en éclairement de l’effet Kerr électronique. Nous poursuivons alors les travaux menés par Loriot et al. en 2009 qui ont montré que l’indice Kerr électronique saturait avant de s’annuler puis de présenter une contribution négative lorsqu’on augmente l’éclairement (inversion du signe pour quelques dizaines de térawatts par centimètre carré). Nous avons alors étendu cette étude en observant à une longueur d’onde de 400 nm (800 nm dans l’étude originale) cette inversion du signe de l’indice Kerr dans l’air.