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Ce manuscrit traite de l'étude métrologique d'un spectromètre Terahertrz (THz), de la caractérisation et de la quantification de produits pulvérulents par spectroscopie THz. Le sujet a été orienté afin de fournir les études préliminaires nécessaires à une thématique visant la détection de pesticides sur les aliments, à savoir la caractérisation métrologique de l'appareil (études de répétabilité, sensibilité...) ainsi que la faisabilité de la quantification de produits et l'application de méthodes chimiométriques lors du prétraitement des spectres. La thèse est ordonnée autour de trois publications. La première publication consiste en une revue de littérature servant à faire le point sur les applications concrètes existant en spectroscopie THz. La seconde porte sur la première partie de notre travail, à savoir la caractérisation métrologique du spectromètre THz sur lequel nous avons effectué nos mesures. Enfin, la troisième porte sur l'aspect quantification de la spectroscopie THz et la possibilité d'appliquer les mêmes principes et techniques chimiométriques qu'en spectroscopie infrarouge. / This manuscript concerns the metrological study of a Terahertz (THz) spectrometer, the characterization and the quantification of powder products by THz spectroscopy. The subject has been aimed to give preliminary analysis to a wider thematic of pesticides detection on aliments, which implies the metrological characterization of the device (repeatability, sensitivity...) and the quantification feasibility of these products and the application of chemometrics methods for spectral pretreatment. The thesis is organized around three publications. The first publication is a literature review, which aims to list but a few of the concrete applications of THz spectroscopy. The second one concerns the metrological characterization of the THz spectrometer we worked on. Lastly, the third one deals with the quantification aspect of THz spectroscopy and the possibility of using the same principles and chemometrics techniques that are used in infrared spectroscopy.

Ultrafast spectroscopy allows us to probe and understand material properties. With it, we can measure phonon-polaritons (optical phonons coupled with light) and the resulting dispersion curve in lithium niobate. Customizing the excitation source in ultrafast measurements can excite phonon modes to large amplitudes, allowing the experimental exploration of the Potential Energy Surface in solids. However, stronger pump fluences and bigger signal isn't always the answer in ultrafast spectroscopy. When sample signals and their nonlinear and mechanisms cannot be distinguished with 1D measurements, simple 2D THz measurements are a great place to start searching for distinct factors as was the case in cadmium tungstate. 2D measurements when paired with modeling and first principles calculations can reveal cutting edge information about exciting materials.

The main objective of this thesis was to bring the first experimental evidence about the spin-Hall magnetoresistance (SMR) in the Terahertz (THz) spectral range. The time-domain THz spectroscopy (TDTS) was chosen as the main method, and we presented a new experimental scheme, which allows us to observe SMR or magnetoresistive effects with similar symmetry at a wide range of THz frequencies very efficiently. We focused on the study of SMR in the bilayers consisting of either a prototypical ferrimagnetic isolator or of heavy metal (FI/HM) and metallic stacks of ferromagnetic CoFeB and heavy metal Pt layer (FM/HM). While SMR shows a rapid decrease already at the lowest THz frequencies (< 1 THz) in the FI/HM structures, the SMR in FM/HM bilayers persists above 30 THz. These observations are then explained by a different mechanism of SMR. The second part of the thesis is devoted to the construction of the new TDTS setup and an easy-to-use model of the THz setup using the Gaussian description of THz radiation. The simulated results have been compared to corresponding experimental measurements using a spintronic THz emitter (STE). The last part of the thesis describes the emission of intensive THz pulses from large-area STE.

No / The terahertz frequency spectrum of pentaerythritol tetranitrate (PETN) is calculated using Discover[1] with the COMPASS[2] force field, CASTEP[3] and PWscf.[4] The calculations are compared to each other and to terahertz spectra (0.3-3 THz) of crystalline PETN recorded at 4 K. A number of analysis methods are used to characterise the calculated normal modes.

This dissertation reports on data acquisition method and the application of world’s first cryogenic apertureless near-field microscope designed for terahertz frequencies. The dissertation briefly summarizes the commonly used data acquisition methods and the existing challenges in applying near-field technology using broadband terahertz sources. We devised, implemented, and validated a novel measurement technique to resolve the challenges. The novel method improves the traditional method by providing the information of the carrier-envelop-phase of the terahertz pulse. The physical properties of WTe₂ microcrystals depend sensitively on the layer number. By applying both the traditional and the novel techniques, we systematically explored the layer-dependent electromagnetic response of mono-layer and few-layer tungsten ditelluride (WTe₂ microcrystals. On tri-layer WTe₂, we discovered the plasmonic response and imaged the real-space pattern of the terahertz plasmon using the novel measurement technique. On bi-layer WTe₂, our measurements support that the band alignment is semi-metallic instead of semi-conducting. Near-field technology at terahertz frequency is sensitive to the Drude behavior of condensed matters. We imaged the electromagnetic response of the transition of cadmium osmate (Cd₂Os₂O₇) crystals from a high temperature metal to a low temperature magnetic insulator. The result is consistent with the temperature dependence in the direct-current conductivity. In the end, the dissertation discusses the theory and simulation of imaging hydrodynamic flow of materials with viscous electron systems via nano-photocurrent technique. In anisotropic material, nano-photocurrent measures the geometrical properties of the Shockley-Ramo auxiliary field or flux. As a result, the nano-photocurrent is a good candidate to detect the boundary layer and vortex flow pattern of a viscous electron system.

No description available.

Many new applications are being proposed and developed for use in the terahertz (THz) frequency region. Similarly, many new materials are being characterized for possible use in this area. Nanostructured forms are of particular interest since they may yield desirable properties, but they remain especially challenging to characterize. This work focuses on the characterization of zinc oxide (ZnO) in bulk and nanowire form. A method for characterizing nanostructures at THz by use of a parallel-plate waveguide (PPWG) is presented. This method is novel in that it is simple, both in theory and practice, and does not require the use of complex measurement techniques such as differential and double modulated terahertz time-domain spectroscopy (THz-TDS). To enable easy evaluation of the quality of the result the maximum deviation in the material response measurement is presented. The dielectric properties of bulk and nanowire ZnO as determined by THz-TDS measurements are reported, and the electrical conductivity extracted from both are presented for comparison. Experimental results are compared to the well established pseudo-harmonic phonon dielectric model. Shortcomings in the pseudo-harmonic phonon model are resolved when coupled with a modified Drude model. This work will enable the determination of THz material properties from nano-scale and very-thin film materials with better reliability and practicality than what has been possible until now.

In this thesis, I present studies in the field of terahertz (THz) spectroscopy. These studies are divided into three areas: Development of a narrowband THz source, the study of carrier transport in metal thin films, and the exploration of coherent dynamics of quasi-particles in semiconductor nanostructures with both broadband and narrowband THz sources. The narrowband THz source makes use of type II difference frequency generation (DFG) in a nonlinear crystal to generate THz waves. By using two linearly chirped, orthogonally polarized optical pulses to drive the DFG, we were able to produce a tunable source of strong, narrowband THz radiation. The broadband source makes use of optical rectification of an ultra-short optical pulse in a nonlinear crystal to generate a single-cycle THz pulse. Linear spectroscopic measurements were taken on NiTi-alloy thin films of various thicknesses and titanium concentrations with broadband THz pulses as well as THz power transmission measurements. By applying a combination of the Drude model and Fresnel thin-film coefficients, we were able to extract the DC resistivity of the NiTi-alloy thin films. Using the narrowband source of THz radiation, we explored the exciton dynamics of semiconductor quantum wells. These dynamics were made sense of by observing time-resolved transmission measurements and comparing them to theoretical calculations. By tuning the THz photon energy near exciton transition energies, we were able to observe extreme nonlinear optical transients including the onset of Rabi oscillations. Furthermore, we applied the broadband THz waves to quantum wells embedded in a microcavity, and time-resolved reflectivity measurements were taken. Many interesting nonlinear optical transients were observed, including interference effects between the modulated polariton states in the sample. / Graduation date: 2012

Pour répondre aux questions que pose la faisabilité d’un dispositif de détection d’explosifsà l’aide de la technologie de spectroscopie térahertz, cette thèse a exploré troisaxes. Le premier a consisté à établir une base de données des signatures spectrales (indiceet absorption) d’une large gamme de matériaux d’intérêt pour ce type d’applications,à partir des données expérimentales que nous avons mesurées par spectroscopie dans ledomaine temporel. Nous avons identifié les matériaux montrant une signature spectralesignificative et nous avons aussi étudié l’effet des matériaux de dissimulation.Dans la seconde partie de ce travail, nous avons conçu et construit un banc de spectroscopieultra-large bande destiné à une meilleure identification spectrale des substances. Nousavons identifié les limites techniques de ce type de banc et donné les pistes pour atteindreles performances désirées.Ensuite, nous avons développé et validé un banc de spectroscopie en réflexion, de typegoniométrique, afin de détecter des signaux térahertz diffusés par des matériaux hétérogènes.Finalement, nous avons étudié les plasmons de surface dans le domaine térahertz, en vuede la détection de très faibles quantités de matière. / This PhD work was performed in view of using terahertz electromagnetic signals forthe detection and identification of dangerous and prohibited substances. In a first stage,a database of the terahertz properties (namely refractive index and absorption) of thesesubstances was created from the measurements we performed using terahertz time-domainspectroscopy. Then a large bandwidth terahertz time-domain set up has been built, togetherwith a goniometric-type set up that allows us recording signals scattered by roughor heterogeneous samples. Finally, we studied the excitation and propagation of surfaceplasmons in the terahertz domain, which may be used for the detection of small amountsof matter.