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In this thesis, we propose and demonstrate a simple and precise method for measuring mm scaled cell gap by using terahertz time domain spectroscopy (THz-TDS) system. This method allows us to measure the cell gap from 15mm to 1.5mm. In addition, the accuracy of measured thickness for the proposed method is also discussed and analyzed. Meanwhile, a nematic liquid crystal BL006 with birefringence as high as 0.27 in THz frequency range and its optical properties of cholesteric liquid crystal (CLC) as mixing chiral materials are investigated and reported. The ordinary refractive index and average effective refractive index at 20oC are from 1.52 to 1.56 and from 1.61 to 1.64, respectively, in THz frequency ranging from 0.2 THz to 1.4THz. In addition, we also demonstrate that cell filled with CLC is with polarization independent property for THz radiation. Through the 5mm cell filled CLC with diluted concentration of the dopant chiral material for decreasing the critical voltage, an electric controlled polarization independent phase shifter with the modulation depth exceeding 2pi is demonstrated. Furthermore, we also investigate the driving field dependence of phase retardation and discuss the reliability.

In this study, suspensions of metallic nanoparticles in base fluids, nanofluids, are investigated by using terahertz time domain spectroscopy (THz-TDS). Nanofluids are used as the working fluid in a variety of applications especially for the purpose of heat transfer enhancement. Polar fluids are being used as the base in nanofluids for their tendency to stop aggregation and sedimentation. Polar fluids highly absorb THz signal. In order to select the best possible host, various polar liquids have been investigated, and isopropanol (99.5%) is selected to be the best candidate for its low THz absorptivity when compared to ethanol (99.5%), ethylene glycol (99%), methanol (95%) and distilled water. Ag, Pd and Cu nanoparticles have been custom-made in isopropanol by laser ablation method, and the size distributions have been characterized by Zeta Potential Analyzer. The nanoparticle diameters are measured to be on average 10 nm, 12 nm and 75 nm for Ag, Cu and Pd, respectively. Nanofluids of 1X, 2X and 3X concentrations of Ag, Cu and Pd nanoparticles have been prepared by diluting with pure (99.5%) isopropanol. Measurements have been repeated after 7 days up to 12 days in order to check for aggregations and sedimentations. THz-TDS is a strong tool to analyze the refractive index and absorption coefficient, but no distinct difference was observed in the frequency domain analysis for the nanofluid samples. On the other hand, in the time domain data analysis, a shift on the time data with a change in transmission was observed. For Ag nanoparticles a positive time shift with a decrease in transmission with increasing concentration was observed. For Cu nanoparticles an interesting negative time shift and an increase in the intensity was observed with increasing concentration. The Pd nanoparticle solution scans showed almost no shift initially, but a negative time shift after a wait period on the order of days. A model of the transmission of the THz pulse through the nanofluid was developed based on transmission/reflection coefficients due to both dielectric and conducting layered media. The model well explains the positive time shift seen with Ag nanoparticle suspensions but fails to explain the shift seen with the Cu nanoparticle suspensions due to the long path length inside the nanofluid. Negative time-shifts can only be explained by decreasing the path length which suggests additional layering inside the nanofluid medium, or assuming that the chemical composition of the isopropanol host has changed with the addition of Cu and/or Pd nanoparticles. The positive time shifts observed with the Ag nanoparticle suspensions allowed for estimating the change in refractive index of the base fluid. From this change, using effective medium theory based on Maxwell-Garnett model, the concentrations of the nanoparticles were estimated. The results agree within an order of magnitude to commercially available nanofluids which are also non-aggregate.

Disertacijos darbo tikslas buvo sukurti ir ištirti puslaidininkinius terahercinių (THz) impulsų emiterius ir detektorius, skirtus sistemoms, naudojančioms 1 μm bangos ilgio femtosekundinę lazerinę spinduliuotę. THz impulsų generavimo ir detektavimo sistema, kurios optoelektroninius puslaidininkinius komponentus aktyvuoja femtosekundiniai lazerio impulsai, yra plačiai taikoma terahercinėje laikinės srities spektroskopijoje. Tradiciškai tokiose sistemose naudojami Ti:safyre femtosekundiniai lazeriai, kurių spinduliuotės bangos ilgis yra ~800 nm. Šios sistemos nėra patogios dėl jų matmenų, nes lazeriai turi sudėtingą kelių pakopų kaupinimo sistemą. Pastaruoju metu THz impulsų generavimui vis dažniau naudojami femtosekundiniai kietakūniai ir šviesolaidiniai lazeriai, kurių spinduliuotės bangos ilgis patenka į artimosios IR spinduliuotės sritį. Tačiau šios sistemos vis dar neturi tinkamos medžiagos fotolaidiems elementams gaminti, kurie būtų žadinami 1 – 1,55 µm bangos ilgio lazeriais. Tokios medžiagos, visų pirmą, turi būti jautrios optinei spinduliuotei, o jų draustinės energijos tarpas turi atitikti žadinamos spinduliuotės fotonų energiją, be to sluoksniai turi pasižymėti didele tamsine varža bei labai trumpomis krūvininkų gyvavimo trukmėmis (~ 1 ps). Šioje disertacijoje yra pateikiami THz impulsų generavimo panaudojus puslaidininkių paviršius ir fotolaidžias antenas rezultatai, žadinant 1 µm bangos ilgio femtosekundiniais lazerio impulsais. / The aim of dissertation was to develop and explore the semiconductor material terahertz (THz) pulse emitters, for Terahertz time–domain spectroscopy (THz–TDS) systems using a 1 μm wavelength femtosecond laser radiation. THz pulse generation and detection using optoelectronic semiconductor components in THz–TDS excited by femtosecond laser pulses become these days a powerful experimental technique. Traditionally, mode-locked Ti:sapphire lasers emitting at the wavelengths ~800 nm are used. However Ti:sapphire lasers require many-stage optical pumping arrangement, the system is quite bulky and complicated. The solution could be the lasers emitting in 1 – 1.55 µm, which can be directly pumped by diode laser bars. Recently, several compact, efficient and cost-effective solid-state and fiber laser systems that generate femtosecond pulses at near-infrared wavelengths have been developed and employed for activating THz–TDS systems. The main obstacle of these systems is the lack of material with appropriate bandgap, high dark resistivity and short (~ ps) carrier lifetimes.

The aim of dissertation was to develop and explore the semiconductor material terahertz (THz) pulse emitters, for Terahertz time–domain spectroscopy (THz–TDS) systems using a 1 μm wavelength femtosecond laser radiation. THz pulse generation and detection using optoelectronic semiconductor components in THz–TDS excited by femtosecond laser pulses become these days a powerful experimental technique. Traditionally, mode-locked Ti:sapphire lasers emitting at the wavelengths ~800 nm are used. However Ti:sapphire lasers require many-stage optical pumping arrangement, the system is quite bulky and complicated. The solution could be the lasers emitting in 1 – 1.55 µm, which can be directly pumped by diode laser bars. Recently, several compact, efficient and cost-effective solid-state and fiber laser systems that generate femtosecond pulses at near-infrared wavelengths have been developed and employed for activating THz–TDS systems. The main obstacle of these systems is the lack of material with appropriate bandgap, high dark resistivity and short (~ ps) carrier lifetimes. / Disertacijos darbo tikslas buvo sukurti ir ištirti puslaidininkinius terahercinių (THz) impulsų emiterius ir detektorius, skirtus sistemoms, naudojančioms 1 μm bangos ilgio femtosekundinę lazerinę spinduliuotę. THz impulsų generavimo ir detektavimo sistema, kurios optoelektroninius puslaidininkinius komponentus aktyvuoja femtosekundiniai lazerio impulsai, yra plačiai taikoma terahercinėje laikinės srities spektroskopijoje. Tradiciškai tokiose sistemose naudojami Ti:safyre femtosekundiniai lazeriai, kurių spinduliuotės bangos ilgis yra ~800 nm. Šios sistemos nėra patogios dėl jų matmenų, nes lazeriai turi sudėtingą kelių pakopų kaupinimo sistemą. Pastaruoju metu THz impulsų generavimui vis dažniau naudojami femtosekundiniai kietakūniai ir šviesolaidiniai lazeriai, kurių spinduliuotės bangos ilgis patenka į artimosios IR spinduliuotės sritį. Tačiau šios sistemos vis dar neturi tinkamos medžiagos fotolaidiems elementams gaminti, kurie būtų žadinami 1 – 1,55 µm bangos ilgio lazeriais. Tokios medžiagos, visų pirmą, turi būti jautrios optinei spinduliuotei, o jų draustinės energijos tarpas turi atitikti žadinamos spinduliuotės fotonų energiją, be to sluoksniai turi pasižymėti didele tamsine varža bei labai trumpomis krūvininkų gyvavimo trukmėmis (~ 1 ps). Šioje disertacijoje yra pateikiami THz impulsų generavimo panaudojus puslaidininkių paviršius ir fotolaidžias antenas rezultatai, žadinant 1 µm bangos ilgio femtosekundiniais lazerio impulsais.

One-dimensional (1D) nanomaterials are of great importance for a number of potential applications. However, in order to realize this potential a thorough understanding of the charge-carrier dynamics in these materials is required, since these largely determine the optoelectronic properties of the materials in question. This thesis investigates the charge-carrier dynamics of two 1D nanomaterials, single-walled carbon nanotubes (CNTs) and tungsten-oxide nanowires (WOxNWs), with the goal of better understanding the nature of their optoelectronic responses, and how nanomaterial geometry and morphology influence these responses. We do this using terahertz time-domain spectroscopy (THz-TDS) and optical pump - terahertz probe time-domain spectroscopy (OPTP). Firstly, we discuss how to properly analyse and interpret the data obtained from these experiments when measuring 1D nanomaterials. While the data obtained from THz-TDS is fairly straight-forward to analyse, OPTP experimental data can be far from trivial. Depending on the relative size of the sample geometry compared to the probe wavelength, various approximations can be used to simplify the extraction of their ultrafast response. We present a general method, based on the transfer matrix method, for evaluating the applicability of these approximations for a given multilayer structure, and show the limitations of the most commonly used approximations. We find that these approximations are only valid in extreme cases where the thickness of the sample is several orders of magnitude smaller or larger than the wavelength, which highlight the danger originating from improper use of these approximations. We then move on to investigate how the charge-carrier dynamics of our CNTs is influenced by nanotube length and density. This is done through studying the nature of the broad THz resonance observed in finite-length CNTs, and how the nanotube length and density affects this resonance. We do this by measuring the conductivity spectra of thin films comprising bundled CNTs of different average lengths in the frequency range 0.3-1000 THz and temperature interval 10-530 K. From this we show that the observed temperature-induced changes in the terahertz conductivity spectra depend strongly on the average CNT length, with a conductivity around 1 THz that increases/decreases as the temperature increases for short/long tubes. This behaviour originates from the temperature dependence of the electron scattering rate, which results in a subsequent broadening of the observed THz conductivity peak at higher temperatures and a shift to lower frequencies for increasing CNT length. Finally, we show that the change in conductivity with temperature depends not only on tube length, but also varies with tube density. We record the effective conductivities of composite films comprising mixtures of WS2 nanotubes and CNTs vs CNT density for frequencies in the range 0.3-1 THz, finding that the conductivity increases/decreases for low/high density films as the temperature increases. This effect arises due to the density dependence of the effective length of conducting pathways in the composite films, which again leads to a shift and temperature dependent broadening of the THz conductivity peak. Next, we investigate the conflicting reports regarding the ultrafast photoconductive response of films of CNTs, which apparently exhibit photoconductivities that can vastly differ, even in sign. Here we observe explicitly that the THz photoconductivity of CNT films is a highly variable quantity which correlates with the length of the CNTs, while the specific type of CNT has little influence. Moreover, by comparing the photo-induced change in THz conductivity with heat-induced changes, we show that both occur primarily due to heat-generated modification of the Drude electron relaxation rate, resulting in a broadening of the plasmonic resonance present in finite-length metallic and doped semiconducting CNTs. This clarifies the nature of the photo-response of CNT films and demonstrates the need to carefully consider the geometry of the CNTs, specifically the length, when considering them for application in optoelectronic devices. We then move on to consider our WOxNWs. We measure the terahertz conductivity and photoconductivity spectra of thin films compromising tungsten-oxide (WOx) nanowires of average diameters 4 nm and 100 nm, and oxygen deficiencies WO2.72 and WO3 using THz-TDS and OPTP. From this we present the first experimental evidence of a metal-to-insulator transition in WOx nanowires, which occurs when the oxygen content is increased from x=2.72 -> 3 and manifests itself as a massive drop in the THz conductivity due to a shift in the Fermi level from the conduction band down into the bandgap. Furthermore we present the first experimental measurements of the photoexcited charge-carrier dynamics of WOx nanowires on a picosecond timescale and map the influence of oxygen-content and nanowire diameter. From this we show that the decay-dynamics of the nanowires is characterized by a fast decay of < 1 ps, followed by slow decay of 3-10 ps, which we attribute to saturable carrier trapping at the surface of the nanowires.

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.

<p dir="ltr">Terahertz Time Domain Spectroscopy (THz-TDS) is a powerful non-destructive, non-ionizing spectroscopic technique utilized for evaluating the optical properties of materials within the terahertz frequency range, spanning from 0.1 to 10 terahertz or wavelengths of 300 micron to 3000 micron. It effectively bridges the gap between microwave and infrared regions on the electromagnetic spectrum and its high resolution which avoiding scattering can quantify small changes in dielectric properties of media. It has high transmission through visibly opaque polymers and its ability to record both magnitude and phase information makes it a strong spectroscopic technique with applications in security, chemistry, electronics and telecommunication and non-destructive evaluation methods for solid mechanics.</p><p><br></p><p dir="ltr">This work introduces a polarization-dependent analytical model employing THz-TDS for computing strain in materials. The model establishes a correlation between volumetric strain and the change in time of arrival for a THz pulse, leveraging dielectrostrictive properties, variations in doping particle density, and changes in sample thickness due to Poisson’s effects. Validation of the analytical model is achieved through strain mapping of polydimethylsiloxane doped with highly dielectrostrictive strontium titanate (STO). Two experiments, including open-hole tensile and circular edge-notch specimens, demonstrate the efficacy of the model. Additionally, the study accounts for stress relaxation behavior to ensure measurement accuracy. Comparison of THz strain mapping results with finite element model (FEM) and surface strain measurements using digital image correlation (DIC) method highlights the technique's sensitivity to material features such as particle clumping and edge effects, while showcasing strong agreement with FEM and DIC results.</p><p><br></p><p dir="ltr">This analytical model is further expanded for experimentally mapping subsurface stress and strain in the adhesive layer of a single lap shear test. This in-situ non-destructive testing method pioneers the use of THz-TDS for stress estimation in the adhesive layer. Validation through strain mapping of STO doped Araldite 2011 epoxy adhesive with the analytical formulation is presented.</p><p dir="ltr">Finally, THz-TDS is applied for fracture front mapping in a double cantilever beam test with high-density polyethylene bonded with STO doped Araldite 2011. The phase-dependent model for mapping fracture fronts in the sub-surface adhesive layer involves analyzing convoluted waves due to interface resonances in a multi-layer structure using THz-TDS in transmission mode. The technique evaluates changes in dielectrostrictive properties and degree of separation to delineate fracture fronts. THz image enhancement algorithms facilitate crack front delineation. Error analysis on measured crack thickness is conducted to evaluate signal-to-noise ratio for THz-TDS. Additionally, an approach employing THz-TDS measured fracture propagation information for determining sub-surface stress maps in the adhesive layer and computing fracture toughness (G_Ic) is proposed. This work highlights the versatility and efficacy of THz-TDS in material characterization and stress/strain mapping in solid mechanics applications.</p>

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.