The goal of this thesis is to describe development of compact terahertz time-domain spectrometer driven by a mode-locked Ti:Sapphire laser. The terahertz radiation was generated by photoconductive antenna method and detected by electro-optic detection method. In this thesis, several terahertz generation and detection method, working principle of terahertz time-domain spectroscopy and its applications are discussed. We mainly focused on working principle of terahertz time-domain spectroscopy and characterization of detected terahertz power using electro-optic detection method.

L’objectif de ma thèse est d’étendre les modèles électromagnétiques existants à l’Institut Fresnel pour les fréquences optiques vers le domaine des fréquences térahertz (THz), pour mieux comprendre les phénomènes physiques mis en jeu lors d’interaction onde-matière. Cette compréhension permettrait d’améliorer l’analyse des images THz acquises et de mieux définir les configurations des systèmes optiques utilisés. Ce travail est réalisé en comparant les résultats issus de la modélisation avec ceux provenant d’expériences menées par imagerie THz au sein de l’entreprise Terahertz Waves Technologies. Dans le futur, la modélisation pourrait devenir un outil prédictif pour la caractérisation de matériaux dans le domaine THz.Les ondes THz se situent entre l’infrarouge lointain et les micro-ondes dans le spectre électromagnétique allant de 0.01 mm à 3 mm (ou 100 GHz à 30 THz). Ces ondes bénéficient des avantages des ondes optiques et des micro-ondes dépendant des longueurs d’ondes utilisées. L’imagerie THz présente un fort potentiel pour la caractérisation de la matière, car ces ondes peuvent pénétrer beaucoup de matériaux qui sont opaques dans le visible et dans l’infrarouge. La détection de défauts, les délaminations, la présence d’humidité, etc…, sont un exemple des problématiques qui peuvent être investiguées grâce au rayonnement THz.Dans un premier temps, j’ai pu simuler la réponse optique d’échantillons polymères plans homogènes et isotropes avec de bons accords entre le calcul et la mesure. Ces résultats ont permis de réaliser de premières modélisations d’images en adéquation avec l’imagerie THz. L’étude est ensuite élargie aux matériaux anisotropes qui existent dans l’environnement industriel actuel ainsi qu’aux objets de forme cylindrique. Les modèles développés considèrent l’indice de réfraction complexe d’un échantillon et son épaisseur, c’est pourquoi un chapitre est dévolu à la méthode d’estimation de ces paramètres à partir de mesures issues de spectroscopie THz dans le domaine temporel mise en œuvre. / The aim of my thesis is to extend the electromagnetic models already existing at the Institut Fresnel for the optical frequencies towards the terahertz (THz) range, to have a better knowledge of the physical phenomena involved in THz light-matter interactions. This understanding would allow to improve the analysis of the THz images acquired and to have a better definition of the optical systems configurations that we use. To achieve this work, we compare the results coming from the model with those from the experiments led by THz imaging by Terahertz Waves Technologies. In the future, the modelling could become a predictive tool for the characterization of materials in the THz domain.THz waves are located between far infrared and microwaves in the electromagnetic spectrum going from 0.01 mm to 3 mm (or 100 GHz to 30 THz). These waves benefit from advantages of the optical waves and from microwaves depending on used frequencies. THz imaging presents a high potential one for the characterization on the material, because these waves can penetrate a lot of materials which are opaque in the visible and the infrared lights. Detection of defects, delaminations, the presence of humidity, etc…, are examples of the problems which can be investigated with THz light.At first, I was able to model the optical response of planar, homogenous, isotropic and polymeric samples with good agreements between the calculation and the measurement. These results allowed to realize first modellings of images which are consistent with THz imaging. Therefore, the study is enlarged to anisotropic materials which exist in the current industrial environment as well as the objects of full cylindrical shape. The developed models consider the complex refractive index of a sample and its thickness, that is why a chapter is devoted to the method of estimation of these parameters from measurements coming from THz Time-Domain Spectrocopy signals which was implemented.

La gamme des ondes terahertz (THz) se situe à l'interface des domaines électronique et optique. Malgré un potentiel d'applications élevé, elle souffre d'un manque de dispositifs performants. Dans ce cadre, cette thèse se concentre sur l'étude fondamentale et la réalisation de nouvelles fonctionnalités associées à différentes sources THz, en utilisant la spectroscopie THz dans le domaine temporel (TDS). Cet outil puissant permet de mesurer le profil temporel d'un champ électrique THz et est utilisé pour explorer l'émission THz de lasers à cascade quantique (LCQ) et de graphène.Dans une première partie, la réponse ultrarapide de LCQs est étudiée. Un contrôle de la phase du champ électrique de LCQs THz via la technique "d'injection seeding" est réalisé puis optimisé. Il nous permet de mesurer le profil temporel de l'émission laser. A l'appui de cette expérience et de simulations, une description quantitative de la dynamique du gain est faite. Ces informations sont critiques pour la production d'impulsions courtes. Une modulation rapide du gain de LCQ est ensuite réalisée et conduit à la génération d'impulsions courtes (durée ~ 15 ps) en régime de blocage de modes. Ces études permettent notamment d'envisager les LCQs comme sources puissantes pour la TDS. Dans une seconde partie, nous montrons que le graphène peut émettre un rayonnement THz sous excitation optique par un effet non linéaire d'ordre 2. Cette émission résulte d'un transfert de quantité de mouvement des photons aux électrons du graphène ("photon drag"). Elle permet ainsi d'explorer des propriétés subtiles du graphène, telles que de très faibles différences de comportement entre les électrons et trous photogénérés. / The terahertz (THz) range is a region of the electromagnetic spectrum which lies at the limit between the electronic and optical domain. Currently, THz applications suffer from the lack of sources and detectors. In this context, this thesis focuses on the fundamental study and the development of new functionalities of different THz sources, usingTHz time-domain spectroscopy (TDS) as a base. This powerful tool enables to acquire the temporal profile of a THz electric field and is used to explore the THz emission properties of quantum cascade lasers (QCLs) and graphene.In the first part, the ultrafast response of QCLs is investigated. A phase control of the electric field of THz QCLs via injection seeding is realised and optimised. This enables the measurement of the amplitude and temporal profile of the laser emission. Throughthese experiments and simulations, a quantitative description of the gain dynamics can be accessed. This information is critical for modelocking. Finally, a fast modulation of the gain of QCLs is realized and leads to short pulses generation (15 ps) in a modelocked regime. These studies open the way for using QCLs as powerful sources in TDS.In the second part, THz radiation generation from graphene under optical excitation is demonstrated by a second order non-linear process. The THz emission results from themomentum transfer from the photons to the electrons of graphene (photon drag). As well as broadband THz generation, novel bandstructure properties of graphene can be explored such as the different dynamics between the photogenerated electrons and holes.

This thesis focuses on improving the performance of the THz time-domain spectroscopy system using second-order nonlinear crystals for THz generation and detection in terms of bandwidth, sensitivity, and THz field strength. The theories for the THz generation based on optical rectification and detection technique, electro-optical sampling, based on Pockels effect are introduced in Chapter 2. In Chapter 3, some experiments are presented to characterize the performances of the THz system based on a 180 fs Yb:KGW femtosecond laser amplifier operating at 1035 nm. The Yb-based femtosecond laser is becoming increasingly popular due to its robustness, high repetition rate, and high average power. However, the NIR bandwidth of these femtosecond lasers is limited by the gain bandwidth of the gain medium, and achieving pulse durations shorter than 180 fs is challenging. Consequently, the full bandwidth of THz time-domain spectroscopy systems is constrained by such laser systems. In order to broaden the THz bandwidth of such THz time-domain spectroscopy systems, our work in Chapter 4 combines the Yb:KGW femtosecond laser amplifier with an argon-filled hollow-core photonic crystal fiber pulse shaper to spectrally broaden the near-infrared pulses from 3.5 to 8.7 THz, increasing the measured THz bandwidth correspondingly from 2.3 THz to 4.5 THz. This is one of the first works to have broadband THz system based on Yb-based femtosecond lasers in the year of 2018. In Chapter 5, the tilted-pulse-front phase matching in the THz generation and detection scheme is demonstrated using the same surface-etched phase gratings on the front surfaces of the 2 mm-thick GaP generation and detection crystals. This scheme overcomes the THz generation and detection bandwidth limit of thick crystals imposed by the traditional collinear phase matching, while allowing the long nonlinear interaction length. This results in a THz spectral range from 0.1 to 6.5 THz with a peak at 3 THz and a peak dynamic range of 90 dB. In the range between 1.1 and 4.3 THz, the system dynamic range exceeds 80 dB. Based on this contact grating-based THz generation, the next step involves generating high-field THz above 2 THz. For high-field THz generation, the most renowned technique is the tilted-pulse-front technique, which generates high-field THz below 2 THz in a LiNbO₃ crystal. Most nonlinear optics experiments in the THz regime rely on such THz sources. To generate high-field THz above 2 THz, one promising candidate is organic THz crystals. However, most organic crystals require a pump laser with a wavelength exceeding 1200 nm, necessitating a more complex laser system. Additionally, the low damage threshold of these crystals are susceptible to compromise the stability of the measurements. Other techniques, such as air plasma and metallic spintronics, can generate ultra-broadband high-field THz from 0.1 to 30 THz, but the pulse energy within certain frequency windows is relatively low, rendering these THz sources less effective for nonlinearly driving specific optical transitions. On the other hand, semiconductor crystals as THz generation crystals, have a high damage threshold and can achieve good phase matching at wavelength around 800 or 1000 nm. In Chapter 6, high-field THz generation with a peak field of 303 kV/cm and a spectral peak at 2.6 THz is achieved with a more homogenous grating on the surface of a 1 mm-thick GaP generation crystal in a configuration collimating the near-infrared generation beam with a pulse energy of 0.57 mJ onto the generation crystal. The experiments also show that the system operates significantly below the GaP damage threshold and THz generation saturation regime, indicating that the peak THz field strength can approach 1 MV/cm, with a 5 mJ near-infrared generation pulse. This is the first high-field THz source based on semiconductor crystals capable of generating high-field THz above 2 THz. With such a THz source, we can conduct nonlinear optics experiments above 2 THz, including the study of phonon-assisted nonlinearities, coherent control of Bose-Einstein condensation of excitons and polaritons in semiconductor cavities, and saturable absorption in molecular gases.

Terahertz time-domain spectroscopy systems were developed and used for the anaylsis and characterization of various materials. By using ultra-fast Ti:Sapphire and Er-doped fiber lasers, terahertz time-domain spectrometers of different configurations were constructed and tested. To increase the accuracy and sensitivity of the measurements, the systems were optimized for spectroscopic analysis. MBE grown nominally undoped epitaxial GaAs samples were used for the spectroscopic measurements. These samples were first charactrized by electrical measurements in order to check the accuracy of the terahertz time-domain experiments. We have shown that the terahertz time-domin spectroscopic techniques provides a quick way of the determining the real ( ) and complex () components of the refractive index of material. In addition, we have investigated the photoexcitation dynamics of these GaAs samples. We have demonstrated that direct and photoexcited terahertz time-domain measurements give an estimate of the carrier densities and both the hole and electron mobility values with good precision. rnin An algorithm is developed to prevent the unwanted Fabry-Perot reflections which is commonly encountered in Terahertz Spectroscopy systems. We have performed terahertz time-domain transmission measurements on ZnTe &lt / 110&gt / crystals of various thicknesses to test the applicability of this algorithm. We have shown that the algorithm developed provides a quick way of eliminating the &ldquo / etalon&rdquo / reflections from the data. In addition, it is also shown that these &ldquo / etalon&rdquo / effects can be used for the frequency calibration of terahertz time-domain spectrometers.

Ce travail de thèse a été réalisé dans le cadre d'un contrat avec l'ANR (ANR-09-VERS-013 « THID ») et porte sur le développement d'une nouvelle génération de tags Chipless à bas coûts fonctionnant dans le domaine THz, pour des applications d'identification et/ou authentification unitaire des articles commerciaux, des papiers d'identités, des personnes pour le contrôle d'accès... Les structures proposées, constituées d'un empilement périodique de couches diélectriques d'indices de réfraction différents, utilisent les propriétés particulières des cristaux photoniques 1D de présenter une réponse électromagnétique entrecoupée de bandes interdites photoniques (BIP). Toute perturbation de la périodicité de la structure engendre des pics dans les bandes interdites qui sont utilisés pour coder une information binaire. Cette structuration particulière des matériaux permet donc de manipuler précisément une signature électromagnétique. Pour des raisons liées à l'industrialisation (facilité de fabrication en masse) et aussi de coût, nous avons retenu des matériaux de base déjà couramment utilisés dans l'industrie papetière : le papier et le polyéthylène. Le choix de ces matériaux, qui doivent allier contraste d'indice élevé et faible absorption, représente une étape cruciale dans ce travail. Ainsi, à partir des résultats expérimentaux obtenus par spectroscopie THz dans le domaine temporel (THz-TDS) sur un grand nombre de matériaux, nous avons pu concevoir deux familles de tags sur la base de ces différents matériaux. Par ailleurs, nous avons développé deux méthodes de codage d'une information binaire, toutes deux basées sur l'absence ou la présence de pics dans une BIP, pics dont la position et le nombre dépendent bien évidemment des défauts de périodicité introduits. Pour des applications liées à l'identification, des capacités de codage de près de 20 bits ont été démontrées. Nous avons aussi montré que la richesse d'information contenue dans la réponse électromagnétique de ces Tags THz peut être utilisée pour les applications liées à l'authentification unitaire, en utilisant comme critère de discrimination le coefficient d'autocorrélation. Nous avons ainsi pu évaluer les performances d'un test d'authentification basé sur ce critère dans différents domaines d'analyse : temporel, fréquentiel et temps-fréquence. Nous avons montré qu'une étude du spectrogramme (combinant temps et fréquence) est ainsi bien plus pertinente qu'une étude dans les seuls domaines temporel ou fréquentiel. / This thesis work deals with the development of a new generation of low-cost Chipless tags operating in the THz frequency domain, it has been supported by the french national agency for research (ANR-09-VERS-013 « THID » ). It covers a wide area of applications such as the identification and/or unitary authentication of commercial items, identity papers, access control…To manufacture these tags, we proposed to use a periodic stack of dielectric material layers with different refractive index and whose thickness is of the order of the wavelength, commonly known as a one dimensional photonic crystal. The electromagnetic signature of such a structure exhibits photonic bandgaps (PBG), i.e. frequency windows in which light propagation is prohibited. We suggested modifying the periodicity of the crystal to create defect levels (peaks) for example in the 1st PBG to encode binary information. This particular structure allows to precisely tuned an electromagnetic signature. To ensure a mass and cost effective industrialization, we retained basic materials which are widely used in the pulp and paper industry: paper and polyethylene. The choice of these materials, which must combine high index contrast and low absorption, represents the first and a crucial step in this work. We characterize a wide range of materials using classical THz time domain spectroscopy (THz-TDS) and we propose two families of tags based on paper and polyethylene. Furthermore, we developed two methods to encode binary information, both based on the absence or presence of peaks in a PBG, peaks whose number and position depend on the introduced defects of periodicity. In a real identification test, a coding capacity of nearly 20-bit has been demonstrated. We also showed that the information contained in the electromagnetic response of these THz tags can be used for other applications related to the unitary authentication and by using the correlation coefficient as criterion for discrimination of the different signatures. Therefore, we evaluate the performance of an authentication test based on this criterion in various analysis domains: time, frequency and time-frequency. We showed that a study of the spectrogram (combining time and frequency representation) is much more relevant than a study in the only time or frequency domain.

This thesis deals with the methods of Terahertz (THz) spectroscopy to observe the kinetics of haemostatic materials used for supporting the native mechanism of haemostasis. The theoretical part follows the physical principles of THz time-domain spectroscopy (THz TDS), mentions the advantages and limitations of this method and its application possibilities for the characterization of biomedical materials. Further, there are specified properties of actual haemostats, described principles of their function and usage in practice, including their interaction with the living tissue. There were performed experiments monitoring the kinetics of physiologic reaction of the tissue adhesive based on the cyanoacrylates and absorbable haemostats. The mechanisms of monitored reactions were explained based on the physical-chemical principles that are used also for the kinetic models’ derivation. Modelling of the measured data results in the estimation of the parameters characterizing the observed samples. The most interesting parameter is the time constant of the reaction because of the possibility to compare reaction rates of different types of haemostats. The detailed analysis of this parameter is performed using the means of statistical methods. Tissue adhesive samples were measured by other spectroscopic and microscopic methods to compare the findings with the experimental results of the THz TDS. Data were processed using algorithms designed especially for this experiment and analysed using mathematical methods.

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