Simple guidelines to predict self-phase modulation patterns

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.

Collisional effects on spectral line shape from the Doppler to the collisional regime: A rigorous test of a unified model

International audience; The paper presents high resolution Raman investigations of the Q(1) line of H-2 in Ar mixture from low density (Doppler regime) to high density (collisional regime) analyzed with a unique line shape profile. Measurements are performed by stimulated Raman gain spectroscopy between 300 and 1000 K in a wide density range (from 0.2 to 11 amagat). All the observed spectral features are accurately described by a unified model recently proposed by two of the authors. This model accounts for a velocity-memory process, not restricted to the usual hard and soft limits. It also includes correlation between velocity- and phase-changing collisions. An exhaustive analysis of vario…

Femtosecond time resolved coherent anti-Stokes Raman spectroscopy: Experiment and modelization of speed memory effects on H2-N2 mixtures in the collision regime

194317; With the aim of temperature diagnostic, femtosecond time-resolved CARS (coherent anti-Stokes Raman spectroscopy) is applied to probe H2 in H2-N2 mixtures. In a first part, a Lorentzian profile is used to model the femtosecond CARS response. A difference between the experimental broadening and the expected one is observed in the collision regime. The observed broadening increases strongly in an inhomogeneous way with respect to the perturber concentration. This is of considerable importance for temperature measurements. In a second part, we show that in the collision regime, this inhomogeneous broadening is due to the speed dependence of the collisional parameters and the memory effe…

Two-wave interferences space-time duality: Young slits, Fresnel biprism and Billet bilens

International audience; Taking advantage of the analogy that can be drawn between the spatial and temporal propagations, we explore two-wave temporal interference in textbook cases such as Young's double slits, Fresnel's biprism and Billet's bilens. We illustrate our approach by numerical simulations for short pulses propagating in dispersive optical fibers with parameters typical of those found in modern optical telecommunications.

Field-free molecular alignment for probing collisional relaxation dynamics

International audience; We report the experimental study of field-free molecular alignment in CO2 gas mixtures induced by intense femtosecond laser pulses in the presence of collisional processes. We demonstrate that the alignment signals exhibit specific features due to nontrivial collisional propensity rules that tend to preserve the orientation of the rotational angular momentum of the molecules. The analysis is performed with a quantum approach based on the modeling of rotational J- and M-dependent state-to-state transfer rates. The present work paves the way for strong-field spectroscopy of collisional dynamics.

H-2 vibrational spectral signatures in binary and ternary mixtures: theoretical model, simulation and application to CARS thermometry in high pressure flames

International audience; A summary of the main results obtained by the two groups in the field of H-2 vibrational spectral line signatures for various mixtures. in connection with CARS diagnostics of H-2-O-2 combustion systems, is presented. H-2-X Systems may have specific large inhomogeneous spectral features, due to the dependence of the line broadening and line shifting on the (H-2) 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 (Besancon). Applications of the present results to high-pressure H-2/air flame thermometry are also briefly…

Molecular alignment in CO2 mixtures induced by a short nonresonant intense pulse : effect of collisional relaxation

The methane Raman spectrum up to 5500 cm-1. Application to the diagnostic of temperature in combustion media

The methane Raman spectrum from 1200 to 5500 cm(-1): A first step toward temperature diagnostic using methane as a probe molecule in combustion systems

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 pr…

Inhomogeneous speed effects on H-2 vibrational line profiles in ternary mixtures

International audience; A study of speed inhomogeneous broadening of the hydrogen vibrational line profiles in the collisional regime for ternary mixtures is reported. The Q(1) line of H-2 in H-2-Ar-N-2, H-2-He-Ar, and H-2-He-N-2 mixtures is investigated by high resolution stimulated Raman spectroscopy for various concentrations and temperatures. A model, successfully used for binary mixtures, is extended to ternary mixtures. An excellent agreement is obtained between theory and experiment for H-2-Ar-N-2, by using the collisional parameters previously obtained from binary mixtures study. For H-2-He-Ar and H-2-He-N-2, H-2-He collisions play a "hardening" effect in the H-2 soft speed memory m…

Dual-broadband rotational CARS modelling of nitrogen at pressures up to 9 MPa. II. Rotational Raman line widths

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 depe…

Optically Probed Laser-Induced Field-Free Molecular Alignment

Molecular alignment induced by laser fields has been investigated in research laboratories for over two decades. It led to a better understanding of the fundamental processes at play in the interaction of strong laser fields with molecules, and also provided significant contributions to the fields of high harmonic generation, laser spectroscopy, and laser filamentation. In this chapter, we discuss molecular alignment produced under field-free conditions, as resulting from the interaction of a laser pulse of duration shorter than the rotational period of the molecule. The experimental results presented will be confined to the optically probed alignment of linear as well as asymmetric top mol…

MOLECULAR LINE-SHAPE MODELING FROM FIRST PRINCIPLES

International audience; We present an ab initio approach to spectral line-shape modeling and the comparison of the results with experimental data.

Experimental and theoretical study of line mixing in methane spectra. III. The Q branch of the Raman nu(1) band

International audience; The shape of the nu(1) Raman Q branch of CH4 perturbed by Ar and He at room temperature has been studied. Stimulated Raman spectroscopy (SRS) experiments have been made in the 2915-2918 cm(-1) spectral region for total pressures from 0.4 to 70 atm and mixtures of approximate to 5% CH4 with He and Ar. Analysis of the spectra demonstrates that the shape of the Q branch is significantly influenced by line mixing and much narrower than what is predicted by the addition of individual line profiles. For the first time, a model is proposed for the calculation and analysis of the effects of collisions on the considered spectra. In this approach, the rotational part of the re…

Optical diagnostic of temperature in rocket engines by coherent Raman techniques

Abstract 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 all…

Impact of a temporal sinusoidal phase modulation on the optical spectrum

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.

Field-free molecular alignment of CO2 mixtures in presence of collisional relaxation

The present work explores the extension of the concept of short-pulse-induced alignment to dissipative environments within quantum mechanical density matrix formalism (Liouville equation) from the weak to the strong field regime. This is illustrated within the example of the CO2 molecule in mixture with Ar and He, at room temperature, for which a steep decrease of the alignment is observed at moderate pressure because of the collisional relaxation. The field-free alignment is measured by a polarization technique where the degree of alignment is monitored in the time domain by measuring the resulting transient birefringence with a probe pulse Raman induced polarization spectroscopy (RIPS) Co…

Field-free molecular alignment in presence of collisional relaxations

Femtosecond Raman Spectroscopy of C2H4 and CH4 molecules

Spectroscopie Raman Anti-Stokes Cohérente femtoseconde (DRASC – fs) : expériences et modélisation dans le cas du mélange H2 – N2 à basse pression

Dans l'objectif du diagnostic de la temperature dans les milieux en combustion, la Diffusion Raman Anti-Stokes Coherente resolue en temps (DRASC - fs) est utilisee pour sonder H 2 dans les melanges H 2 -N 2 a basse pression. Le dispositif DRASC mis en place est decrit en detail. Un nouveau modele de la reponse DRASC temporelle, prenant en compte tous les effets collisionnels specifiques a l'hydrogene (effets dits « de vitesse ») est presentee, ainsi que la comparaison avec l'experience, l'accord se revelant tres satisfaisant.

Speed-memory effects in H2-N2 mixtures studied by CARS femtosecond. Experiments and modelization from the collisional to the Doppler regime

Impact of initial pulse shape on the nonlinear spectral compression in optical fibre

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.

CARS spectroscopy of CH4 for implication of temperature measurements in supercritical LOX/CH4 combustion

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 …

Dissipation of post-pulse laser-induced alignment of CO2through collisions with Ar

In this paper, laser-induced field-free alignment of CO2 in mixtures with Ar is investigated under dissipative conditions (up to 15 bars) at room temperature. The degree of alignment is temporally monitored by a polarization spectroscopy technique, where a weak probe pulse measures the transient birefringence resulting from the alignment. The data are analyzed with a quantum mechanical density matrix formalism using properly J-dependent and M-dependent state-to-state transfer rates, which was previously successfully tested on pure CO2 and CO2–He mixtures. The same consistency is obtained between experiments and calculations, in particular the decay times of both the transient revivals and t…

Experimental and theoretical study of line mixing in methane spectra. III. The Q branch of the Raman ν1 band

The shape of the ν1 Raman Q branch of CH4 perturbed by Ar and He at room temperature has been studied. Stimulated Raman spectroscopy (SRS) experiments have been made in the 2915–2918 cm−1 spectral region for total pressures from 0.4 to 70 atm and mixtures of ≈5% CH4 with He and Ar. Analysis of the spectra demonstrates that the shape of the Q branch is significantly influenced by line mixing and much narrower than what is predicted by the addition of individual line profiles. For the first time, a model is proposed for the calculation and analysis of the effects of collisions on the considered spectra. In this approach, the rotational part of the relaxation matrix is constructed, with no adj…

Rotational CARS thermometry at high temperature (1800 K) and high pressure (0.1-1.55 MPa)

International audience; Dual-broadband rotational CARS (DB-RCARS) thermometry has been investigated at high temperature and high pressure. Single-shot measurements were performed at 1800 K, in air and nitrogen at pressures up to 1.55 MPa and in oxygen at pressures up to 0.5 MPa. For all conditions, the resonant signal contribution to the spectra clearly dominated over the non-resonant one, implying the high potential for DB-RCARS for temperature and concentration measurements also at the high temperatures and pressures used in the present investigation. The relative standard deviation was generally similar to 2% for single-shot data at pressures from 0.5 to 1.55 MPa. At the investigated tem…

Optical Diagnostics with Ultrafast and Strong Field Raman Techniques

In this chapter, we will discuss some coherent techniques, namely Raman Induced Polarization Spectroscopy (RIPS) and femtosecond Coherent Raman Anti-Stokes Spectroscopy (fs-CARS). We will demonstrate their ability to be used as non-invasive optical diagnostic tools for temperature, density, or concentration measurements, as well as a means of testing collision induced energy transfer models (in a low field regime), and studying the so-called inhomogeneous lineshape effects that are particularly enhanced in the case of hydrogen. We will also show how molecular alignment achieved in a strong field regime can provide additional information about collisional relaxation processes. In all cases, …

Speed-dependent line profile: A test of a unified model from the Doppler to the collisional regime for molecule-molecule collisions

International audience; A speed-dependent line profile combining soft and hard fully correlated Dicke-narrowing collisions was recently successfully tested on Ar-broadened H-2 spectra in a wide density and temperature range. A further test for mixtures of H-2 in nitrogen molecules (instead of Ar atoms) is presented. This test is also based on high resolution Raman investigation of the isotropic Q(1) line of H-2 from low to high density at various temperatures. The same consistency of the speed-dependent line profile as for H-2-Ar is obtained for H-2-N-2 through a remarkable agreement with all the data by using a unique set of four parameters (the collisional width and shift, the kinetic fre…

CARS methane spectra: Experiments and simulations for temperature diagnostic purposes

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…