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. / 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).

This thesis explores and expands upon theoretical means of quantifying a number of nonlinear spectroscopies, including two-photon absorption, resonant-inelastic x-ray scattering, Jones birefringence, and magnetic circular dichroism. On top of that, detailed information is given for the derivation and program implementation of damped cubic response functions. Complex-valued cubic response functions have been implemented in the quantum chemistry package DALTON, based on working equations formulated for an approximate-state wave function. An assessment of the implementation, such that for small frequencies the second-order hyperpolarizability should behave according to an analytic function that depends quadratically on the optical frequencies. It is demonstrated how two-photon absorption (TPA) can be described either through second-order transition moments or via the damped cubic response function. A few calculated TPA profiles are produced for a set of smaller molecules, in order to display the capability of the cubic response function in the x-ray frequency region. Resonance-inelastic x-ray scattering (RIXS) is explored in a similar manner as two-photon absorption. It is shown how the second-order hyperpolarizability can represent RIXS in the limit of intermediate-state and final-state resonances. Complications emerging from the complex dispersion of the hyperpolarizability are discussed. Moreover, linear birefringences, with focus on the Jones birefringence, are investigated for noble gases, monosubstituted benzenes, furan homologues, and a pure acetonitrile liquid. A linear relation between the Jones birefringence and the empirical para-Hammett constant as well as the permanent electric dipole moment is presented. Estimations of three linear birefringences --- Kerr, Cotton--Mouton, and Jones ---are obtained by averaging over a set of liquid snapshots. The Jones effect for acetonitrile turns out to be unusually large inmparison to the other two investigated linear birefringences. The final chapter of the thesis investigates magnetically induced circular dichroism (MCD). A question regarding relative stability of the first set of excited states for DNA-related molecular systems is resolved through MCD by exploiting the signed nature of circular dichroisms. Furthermore, to what extent solvent contributions affect MCD spectra is explored. The effect on uracil MCD spectrum due to thionation is studied, for which the degree of redshifting for systems 2-thiouracil and 4-thiouracil can be seen to be addative as compared to the 2,4-dithiouracil system. / <p>QC 20171129</p>

This master's thesis deals with the analysis of the optical power measurement using an optical fiber sensor. The thesis contains the theoretical background to understand the origin of polarization and its representation in space using Poincaré’s sphere and Stokes vectors. There is also a part describing optical performance measurement and the preview of analog measurements from various researches. Practical part focuses on verification of changes of fiber sensor parameters at temperature change in its surroundings and this part includes also additional suggestions for various types of measurements and verification of the function of the photodiode as an optical power transducer. Most measurements are based on the comparison of results obtained with the polarimeter. The results were plotted and discussed.

The thesis deals with integral and distributed optical fiber sensors of electric current. In the area of integral sensors the analysis is performed by Jones matrix calculus and the simultaneous influence of induced circular and undesired linear birefringence using an ortho-conjugation retroreflector. Furthermore, the proposed conjugation loop variant using half-wave phase retarders is analyzed. The theoretical conclusions are confirmed by simulation and experimental measurement. In the field of distributed fiber optic sensors, analysis and simulation for the detection of plasma currents in thermonuclear fusion reactors, based on the POTDR technique, is performed. An improvement procedure is proposed for circular-shaped vacuum vessel reactors. Plasma current detection procedure in divertor-type reactors have been newly designed and simulated to investigate the effect of the OTDR detector noise on plasma current detection accuracy.

L'interférométrie visible longue base est une technique d'observation en astronomie permettant de sonder les objets avec une résolution spatiale qu'il est impossible d'atteindre avec un télescope seul. La mise en œuvre au sol de cette méthode est limitée en sensibilité et précision de mesure à cause de la turbulence atmosphérique. Or les nouveaux besoins scientifiques, tels que la détermination des paramètres fondamentaux, l'étude de l'environnement proche ou de la surface des étoiles, requièrent la capacité d'observer des objets de moins en moins brillants et de faire des mesures de plus en plus précises, en interférométrie visible. Pour s'affranchir de la turbulence, l'interférométrie multimode a été développée en reprenant le concept de l'interférométrie des tavelures utilisée sur un seul télescope. Aujourd'hui, pour améliorer davantage les performances des futurs instruments, cette instrumentation évolue vers l'utilisation de la nouvelle génération de détecteur, l'Electron Multiplying Charge-Coupled Device (EMCCD), et de l'emploi des fibres optiques interfacées avec des optiques adaptatives. Cette avancée est motivée par le succès de l'utilisation conjointe de l'optique adaptative et du suivi de franges pour s'affranchir partiellement de la turbulence en interférométrie infrarouge, en 2017 avec l'instrument GRAVITY (Gravity Collaboration et al. 2017). Le prototype FRIEND (Fibered and spectrally Resolved Interferometer - New Design) a été conçu pour caractériser et évaluer les performances de la combinaison de ces éléments, dans le domaine visible. L'amélioration de la précision des instruments interférométriques est apportée par les fibres optiques et par la dynamique du signal délivré par une EMCCD. L'inconvénient de l'emploi des fibres dans le visible est une perte de la sensibilité du fait que le taux d'injection du flux dans celles-ci est très faible à cause de la turbulence atmosphérique. Mais il se trouve que l'optique adaptative et l'EMCCD permettent d'améliorer la sensibilité. En effet, l'optique adaptative maximise l'injection en réduisant l'influence de la turbulence atmosphérique, et l'EMCCD est capable de détecteur de faibles flux. FRIEND prépare ainsi le développement du futur instrument SPICA, recombinant jusqu'à six télescopes (Mourard et al. 2017, 2018). Celui-ci devra explorer la stabilisation des interférences grâce au suivi de franges. Cet aspect n'est pas abordé dans cette thèse. Je présente dans cette thèse le prototype FRIEND, capable de recombiner jusqu'à trois télescopes, opérant dans la bande R en franges dispersées. Il est doté de fibres optiques gaussiennes monomodes à maintien de polarisation et d'une EMCCD. Il est installé sur l'interféromètre visible Center for High Angular Resolution Astronomy (CHARA), au Mount Wilson, en Californie, qui est en train de s'équiper d'optiques adaptatives. J'ai développé des estimateurs de visibilité et de clôture de phase, la méthode de réduction des données de ce prototype et une stratégie d'observation. Grâce à ces outils, j'ai montré que les optiques adaptatives améliorent le taux d'injection dans les fibres. Il est alors apparu que la stabilisation de l'injection est importante pour maximiser le rapport signal-à-bruit dans chaque image. La biréfringence des fibres dégrade les performances de l'instrument mais elle a pu être compensée. J'ai montré qu'un instrument, basé sur la conception de FRIEND, permet d'accéder à des mesures de visibilité faibles avec une précision, inatteignable avec la génération actuelle, grâce au développement et l'utilisation d'un modèle de rapport signal-à-bruit. L'instrument a enfin été testé dans son intégralité sur le système binaire connu ζ Ori A. Cette observation montre la fiabilité et la précision des mesures interférométriques obtenues avec ce prototype, montrant l'intérêt de cette association de technologies pour les futurs interféromètres visibles. / Long baseline visible interferometry in astronomy is an observing technique which allows to get insights of an object with an outstanding angular resolution, unreachable with single-dish telescope. Interferometric measurements with ground-based instrumentation are currently limited in sensitivity and precision due to atmospheric turbulence. However, the new astrophysical needs, particularly the determination of fundamental parameters or the study of the closed environment and the surface of the stars, require to observe fainter objects with a better precision than now in visible interferometry. Ought to overcome the atmospheric turbulence, multispeckle interferometry has been developed by adapting speckle imaging technics used on single-dish telescope. Today, in order to improve the performance of the future combiners, instrumentation progresses to the use of a new generation detector called EMCCD, and the use of optical fibers which are coupled with adaptive optics. This path is chosen thank to the success of the use of the adaptive optics with the fringe tracking in the infrared interferometry in 2017 (Gravity Collaboration et al. 2017), in order to compensate turbulence. FRIEND prototype (Fibered and spectrally Resolved Interferometer - New Design) has been designed to characterize and estimate the performance of such a combination of technologies, in the visible spectral band. The improvement of the precision of the measurements from interferometric instruments is due to optical fibers and the dynamical range of the EMCCD. The counterpart of using the optical fibers is a loss in sensitivity due to a low injection rate of flux into the fibers because of the atmospheric turbulence. On the other hand, sensitivity is improved thanks to adaptive optics and EMCCDs. Indeed, adaptive optics increases the injection rate and EMCCDs can measure low fluxes. Lastly, FRIEND is a pathfinder for the future instrument SPICA which should recombine up to 6 telescopes (Mourard et al. 2017, 2018). Fringe-tracking aspects will have to be studied for SPICA; this topic is not dealt with in this thesis. In this work, I present the FRIEND prototype, which can recombine up to three telescopes and operates in the R band with dispersed fringes. It has Gaussian polarization-maintaining single mode optical fibers and an EMCCD. It is set up at the Center for High Angular Resolution Astronomy (CHARA), at Mount Wilson, in California. CHARA is currently being equipped with adaptive optics. I develop estimators of visibility modulus and closure phase, the data reduction software and an observing strategy. Thanks to that, I am able to show that adaptive optics improves the injection rate. I also demonstrate how important the stabilization of injection is to maximize the signal-to-noise ratio (SNR) per frame. Birefringence of the fibers decreases the performance of the instrument but we manage to compensate it. I show how such an instrument can measure low visibility with a better precision than now by developing and using a SNR model of FRIEND. Finally, FRIEND has entirely been tested on the known binary system ζ Ori A. These observations demonstrate how reliable and accurate the measurements of FRIEND are.

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Thin-film-transistor (TFT) liquid crystal display (LCD) has been widely used in smartphones, pads, laptops, computer monitors, and large screen televisions, just to name a few. A great deal of effort has been delved into wide viewing angle, high resolution, low power consumption, and vivid color. However, relatively slow response time and low transmittance remain as technical challenges. To improve response time, several approaches have been developed, such as low viscosity liquid crystals, overdrive and undershoot voltage schemes, thin cell gap with a high birefringence liquid crystal, and elevated temperature operation. The state-of-the-art gray-to-gray response time of a nematic LC device is about 5 ms, which is still not fast enough to suppress the motion picture image blur. On the other hand, the LCD panel's transmittance is determined by the backlight, polarizers, TFT aperture ratio, LC transmittance, and color filters. Recently, a fringe-field-switching mode using a negative dielectric anisotropy (Δε) LC (n-FFS) has been demonstrated, showing high transmittance (98%), single gamma curve, and cell gap insensitivity. It has potential to replace the commonly used p-FFS (FFS using positive Δε LC) for mobile displays. With the urgent need of submillisecond response time for enabling color sequential displays, polymer-stabilized blue phase liquid crystal (PS-BPLC) has become an increasingly important technology trend for information display and photonic applications. BPLCs exhibit several attractive features, such as reasonably wide temperature range, submillisecond gray-to-gray response time, no need for alignment layer, optically isotropic voltage-off state, and large cell gap tolerance. However, some bottlenecks such as high operation voltage, hysteresis, residual birefringence, and slow charging issue due to the large capacitance, remain to be overcome before their widespread applications can be realized. The material system of PS-BPLC, including nematic LC host, chiral dopant, and polymer network, are discussed in detail. Each component plays an essential role affecting the electro-optic properties and the stability of PS-BPLC. In a PS-BPLC system, in order to lower the operation voltage the host LC usually has a very large dielectric anisotropy (Δε > 100), which is one order of magnitude larger than that of a nematic LC. Such a large Δε not only leads to high viscosity but also results in a large capacitance. High viscosity slows down the device fabrication process and increases device response time. On the other hand, large capacitance causes slow charging time to each pixel and limits the frame rate. To reduce viscosity, we discovered that by adding a small amount (~6%) of diluters, the response time of the PS-BPLC is reduced by 2X-3X while keeping the Kerr constant more or less unchanged. Besides, several advanced PS-BPLC materials and devices have been demonstrated. By using a large Δε BPLC, we have successfully reduced the voltage to <10V while maintaining submillisecond response time. Finally we demonstrated an electric fieldindeced monodomain PS-BPLC, which enables video-rate reflective display with vivid colors. The highly selective reflection in polarization makes it promising for photonics application. Besides displays in the visible spectral region, LC materials are also very useful electro-optic media for near infrared and mid-wavelength infrared (MWIR) devices. However, large absorption has impeded the widespread application in the MWIR region. With delicate molecular design strategy, we balanced the absorption and liquid crystal phase stability, and proposed a fluoro-terphenyl compound with low absorption in both MWIR and near IR regions. This compound serves as an important first example for future development of low-loss MWIR liquid crystals, which would further expand the application of LCs for amplitude and/or phase modulation in MWIR region.

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