This project evaluates the ability of terahertz (THz) radiation to differentiate cancerous from non-cancerous human breast lumpectomy and mastectomy tissue. This is done by aiming a narrow-band THz beam at medical samples and measuring reflected power. THz images of specimens from Breast Conservation Surgery (BCS) were created using a gas laser source and mechanical scanning. The design and characterization of this system is discussed in detail. The images were correlated with optical histological micrographs of the same specimens and discrimination values of more than 70% were found for five of the six samples using Receiver Operating Characteristic (ROC) analysis.

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.

No description available.

No description available.

<p>Future wireless applications will require networks to provide high rates, reduced power consumption, reliable communications, and low latencies in a wide range of deployment scenarios. To support the never-ending growth in wireless data traffic, a solution is to operate wireless networks on the wide bandwidth available at higher frequencies, e.g., millimeter wave (mmWave) and sub-terahertz (sub-THz) bands. However, new challenges arise as networks operating at higher frequencies experience harsher propagation characteristics. To compensate for such severe signal attenuation, the directional beamforming via massive multipleinput multiple-output (MIMO) is adopted to provide array gains, but it necessitates accurate MIMO channel state information incurring unacceptably large training overhead. Wireless system engineers will require to develop fast and efficient channel training algorithms for massive MIMO systems. Another new challenge arises in scenarios without a direct link between the source and destination due to serious pathloss, which requires cooperative relay beamforming to enhance the communication coverage. The beamforming weights of the distributed relays and the receive combiner can be jointly optimized to enhance Quality-of-Service in multi-user relay beamforming networks. Our contributions cover three specific topics as follows: First, we develop a learning-based beam alignment approach, which enables the position-aided beam recommendation to support users at new positions, to reduce the training overhead in MIMO systems. Second, we propose a compressed training framework to estimate the time-varying sub-THz MIMO-OFDM channels with dual-wideband effect. Lastly, we propose a joint relay beamforming and receive combiner design, considering an optimization problem formulation that maximizes the minimum of the receiving signal-to-interference-plus-noise ratios among multiple users. In each specific topic, we provide the algorithms and show the numerical results to demonstrate the improved performance over the state-of-the-art techniques.</p>

L’objectif de cette thèse était d’appliquer des méthodes d’analyse multivariées au traitement des données provenant de la spectroscopie de plasma induit par laser (LIBS) et de la spectroscopie térahertz (THz) dans le but d’accroître les performances analytiques de ces techniques.Les spectres LIBS provenaient de campagnes de mesures directes sur différents sites géologiques. Une approche univariée n’a pas été envisageable à cause d’importants effets de matrices et c’est pour cela qu’on a analysé les données provenant des spectres LIBS par réseaux de neurones artificiels (ANN). Cela a permis de quantifier plusieurs éléments mineurs et majeurs dans les échantillons de sol avec un écart relatif de prédiction inférieur à 20% par rapport aux valeurs de référence, jugé acceptable pour des analyses sur site. Dans certains cas, il a cependant été nécessaire de prendre en compte plusieurs modèles ANN, d’une part pour classer les échantillons de sol en fonction d’un seuil de concentration et de la nature de leur matrice, et d’autre part pour prédire la concentration d’un analyte. Cette approche globale a été démontrée avec succès dans le cas particulier de l’analyse du plomb pour un échantillon de sol inconnu. Enfin, le développement d’un outil de traitement par ANN a fait l’objet d’un transfert industriel.Dans un second temps, nous avons traité des spectres d’absorbance terahertz. Ce spectres provenaient de mesures d’absorbance sur des mélanges ternaires de Fructose-Lactose-acide citrique liés par du polyéthylène et préparés sous forme de pastilles. Une analyse semi-quantitative a été réalisée avec succès par analyse en composantes principales (ACP). Puis les méthodes quantitatives de régression par moindres carrés partiels (PLS) et de réseaux de neurons artificiels (ANN) ont permis de prédire les concentrations de chaque constituant de l’échantillon avec une valeur d’erreur quadratique moyenne inférieure à 0.95 %. Pour chaque méthode de traitement, le choix des données d’entrée et la validation de la méthode ont été discutés en détail. / The aim of this work was the application of multivariate methods to analyze spectral data from laser-induced breakdown spectroscopy (LIBS) and terahertz (THz) spectroscopy to improve the analytical ability of these techniques.In this work, the LIBS data were derived from on-site measurements of soil samples. The common univariate approach was not efficient enough for accurate quantitative analysis and consequently artificial neural networks (ANN) were applied. This allowed quantifying several major and minor elements into soil samples with relative error of prediction lower than 20% compared to reference values. In specific cases, a single ANN model didn’t allow to successfully achieving the quantitative analysis and it was necessary to exploit a series of ANN models, either for classification purpose against a concentration threshold or a matrix type, or for quantification. This complete approach based on a series of ANN models was efficiently applied to the quantitative analysis of unknown soil samples. Based on this work, a module of data treatment by ANN was included into the software Analibs of the IVEA company. The second part of this work was focused on the data treatment of absorbance spectra in the terahertz range. The samples were pressed pellets of mixtures of three products, namely fructose, lactose and citric acid with polyethylene as binder. A very efficient semi-quantitative analysis was conducted by using principal component analysis (PCA). Then, quantitative analyses based on partial least squares regression (PLS) and ANN allowed quantifying the concentrations of each product with a root mean square error (RMSE) lower than 0.95 %. All along this work on data processing, both the selection of input data and the evaluation of each model have been studied in details.

Zum ersten Mal konnte die kohärente Erzeugung von ultrakurzen Pulsen mit Feld stärken im MV/cm Bereich mit einem Spektralbereich von 0.1-30 THz im organischen Kristall DSTMS. Kohärente mehrdimensionale Terahertzspektroskopie (CMTS) hat sich zu einer wichtigen Methode zur Untersuchung der niederenergetischen Anregungen von Halbleitern and deren kohärenter Dynamik entwickelt. Eine neuartige CMTS Methode mit drei phasenstarren, zueinander zeitverzögerten Terahertzpulsen wurde entwickelt. Sie beruht auf der kollinearen Wechselwirkung der Pulse mit der Probe, sodass verschiedene Ordnungen des nichtlinearen Signals in gleicher Richtung emittiert werden und deshalb gleichzeitig gemessen werden können. Amplitude und Phase des nichtlinearen Signals können durch elektro-optisches Abtasten vermessen werden, wodurch die zeitliche Entwicklung der kohärenten Wechselwirkungen in Echtzeit untersucht werden kann. CMTS erlaubt zusätzlich die eindeutige Zerlegung des nichtlinearen Signals in die verschiedenen nichtlinearen Ordnungen in der jeweiligen mehrdimensionalen Frequenzdomäne. Die nichtlineare, nicht-resonante Antwort zweier undotierter Halbleiter, des Ferroelektrikums Lithiumniobat (LiNbO3) und Indiumantimonids (InSb) kann mit dieser neuartigen Methode untersucht werden. In LiNbO3 wird das nichtlineare Signal durch einen Femtosekunden nichtlinearen Verschiebestrom (SC) hervorgerufen. SC wird durch die gebrochene Inversionssymmetrie des Kristalls in Verbindung mit einer ultraschnellen Dephasierung der feldinduzierten, kohärenten interband-Polarisation hervorgerufen. Die Dephasierung der interband-Polarisation erlaubt das Tunneln von Elektronen vom Valenzband in das Leitungsband. In InSb wird das kohärente Signal durch sowohl zwei-Phonen als auch zwei-Photonen interband-Anregungen erzeugt. Die impulsive Anregung einer kohärenten zwei-Phononen Polarisation wird durch das große Übergangsdipolmoment von InSb verstärkt, was zu deutlich größeren Amplituden der Polarisation als im linearem Regime führt. / For the first time, the coherent generation of ultrashort MV/cm field pulses with a spectrum covering the frequency range 0.1-30 THz is demonstrated in the organic crystal DSTMS. Coherent multidimensional terahertz spectroscopy (CMTS) has become a prominent technique for, e.g., driving low-energy excitations in semiconductors and monitoring their coherent dynamics. A novel CMTS technique using three phase-locked inter-delayed THz pulses is implemented. It relies on a collinear interaction of the pulses with a sample, so that different contributions to the nonlinear signal are emitted in the same direction, and thus can be measured all at once. Phase-resolved detection by electro-optic sampling allows for measuring amplitude and absolute phase of the nonlinear signal, thereby enabling to investigate the evolution of coherent interactions between quantum excitations in real time. In CMTS, the nonlinear signal is dissected into the distinct nonlinear contributions in the corresponding multidimensional frequency domain. This novel technique is applied to study the nonlinear off-resonant response of two undoped bulk semiconductors, the wide-bandgap ferroelectric lithium niobate (LiNbO3) and the narrow-bandgap indium antimonide (InSb). In LiNbO3, the nonlinear signal is generated by a femtosecond nonlinear shift current (SC), a distinctive characteristic of the bulk photovoltaic effect. The SC stems from the lack of inversion symmetry and the ultrafast dephasing of the field-induced interband coherent polarization due to a sufficiently high decoherence rate, which enables tunneling of electrons from the valence to the conduction band. In InSb, the nonlinear signal is caused by the coherent response on both the two-phonon and two-photon interband excitations. The impulsive generation of the two-phonon coherent polarization is enhanced by the large interband transition dipole of InSb, resulting in much larger polarization amplitudes than in the regime of linear response.

In dieser Arbeit werden niederfrequente optische Messungen an vier neuartigen Supraleitern vorgestellt. Im Bereich von 100 GHz bis 3 THz zeigen die vier untersuchten Systeme – LuNi2B2C, Ba(Fe0,9Co0,1)2As2, T’-Pr2CuO4 und Si:Ga – ein sehr unterschiedliches Verhalten. Die beiden erst genannten Supraleiter sind Mehrbandsupraleiter, bei denen die Cooper-Paarkopplung unterschiedlich für verschiedene Fermiflächen ist. T’-Pr2CuO4 ist ein undotierter Kupratsupraleiter, der nach bisheriger Lehrmeinung nicht existieren dürfte. Mit THz-Spektroskopie konnte erstmals die Bildung einer Meißner-Phase in T’-Pr2CuO4 mit optischen Methoden beobachtet werden. Eine gewisse Sonderstellung nimmt Si:Ga als amorpher Supraleiter ein. Si:Ga wird durch Ionenimplantation von Gallium in einen Siliziumwafer hergestellt. Es besteht die Hoffnung, mit Si:Ga halb- und supraleitende Logikblöcke in großem Maßstab auf einem Chip vereinen zu können, da die Ionenimplantation mit den Produktionsprozessen der Halbleiterindustrie kompatibel ist.

This thesis investigates the use of high-power lasers for synchrotron radiation sources with high brilliance, from the EUV to the hard X-ray spectral range. Hereby lasers accelerate electrons by laser-wakefield acceleration (LWFA), act as optical undulators, or both. Experimental evidence shows for the first time that LWFA electron bunches are shorter than the driving laser and have a length scale comparable to the plasma wavelength. Furthermore, a first proof of principle experiment demonstrates that LWFA electrons can be exploited to generate undulator radiation. Building upon these experimental findings, as well as extensive numerical simulations of Thomson scattering, the theoretical foundations of a novel interaction geometry for laser-matter interaction are developed. This new method is very general and when tailored towards relativistically moving targets not being limited by the focusability (Rayleigh length) of the laser, while it does not require a waveguide. In a theoretical investigation of Thomson scattering, the optical analogue of undulator radiation, the limits of Thomson sources in scaling towards higher peak brilliances are highlighted. This leads to a novel method for generating brilliant, highly tunable X-ray sources, which is highly energy efficient by circumventing the laser Rayleigh limit through a novel traveling-wave Thomson scattering (TWTS) geometry. This new method suggests increases in X-ray photon yields of 2-3 orders of magnitudes using existing lasers and a way towards efficient, optical undulators to drive a free-electron laser. The results presented here extend far beyond the scope of this work. The possibility to use lasers as particle accelerators, as well as optical undulators, leads to very compact and energy efficient synchrotron sources. The resulting monoenergetic radiation of high brilliance in a range from extreme ultraviolet (EUV) to hard X-ray radiation is of fundamental importance for basic research, medical applications, material and life sciences and is going to significantly contribute to a new generation of radiation sources and free-electron lasers (FELs).

Die vorliegende Arbeit beschäftigt sich in Experiment und Theorie mit Laser-Plasma beschleunigten Elektronen und optischen Undulatoren zur Erzeugung von brillianter Synchrotronstrahlung. Zum ersten Mal wird experimentell nachgewießen, dass laserbeschleunigte Elektronenpulse kürzer als 30 fs sind. Ferner werden solche Elektronenpulse erstmalig in einem Demonstrationsexperiment durch einen magnetischen Undulator als Synchrotronstrahlenquelle genutzt. Aufbauend auf diesen experimentellen Erkenntnissen, sowie umfangreichen numerischen Simulationen zur Thomsonstreuung, werden die theoretischen Grundlagen einer neuartigen Interaktionsgeometrie für Laser-Materie Wechselwirkungen entwickelt. Diese neue, in der Anwendbarkeit sehr allgemeine Methode basiert auf raum-zeitlicher Laserpulsformung durch nichtlineare Winkeldispersion wie diese durch VLS- (varied-line spacing) Gitter erzeugt werden kann und hat den Vorteil nicht durch die Fokussierbarkeit des Lasers (Rayleighlänge) begrenzt zu sein. Zusammen mit laserbeschleunigten Elektronen ermöglicht dieser traveling-wave Thomson scattering (TWTS) benannte Ansatz neuartige, nur auf optischer Technologie basierende Synchrotronstrahlenquellen mit Zentimeter bis Meter langen optische Undulatoren. Die hierbei mit existierenden Lasern erzielbaren Brillianzen übersteigen diese bestehender Thomsonquellen-Designs um 2-3 Größenordnungen. Die hier vorgestellten Ergebnisse weisen weit über die Grenzen der vorliegenden Arbeit hinaus. Die Möglichkeit Laser als Teilchenbeschleuniger und auch optischen Undulator zu verwenden führt zu bauartbedingt sehr kompakten und energieeffizienten Synchrotronstrahlungsquellen. Die hieraus resultierende monochromatische Strahlung hoher Brillianz in einem Wellenlängenbereich von extremen ultraviolett (EUV) zu harten Röntgenstrahlen ist für die Grundlagenforschung, medizinische Anwendungen, Material- und Lebenswissenschaften von fundamentaler Bedeutung und wird maßgeblich zu einer neuen Generation ultrakurzer Strahlungsquellen und freien Elektronenlasern (FELs) beitragen. / This thesis investigates the use of high-power lasers for synchrotron radiation sources with high brilliance, from the EUV to the hard X-ray spectral range. Hereby lasers accelerate electrons by laser-wakefield acceleration (LWFA), act as optical undulators, or both. Experimental evidence shows for the first time that LWFA electron bunches are shorter than the driving laser and have a length scale comparable to the plasma wavelength. Furthermore, a first proof of principle experiment demonstrates that LWFA electrons can be exploited to generate undulator radiation. Building upon these experimental findings, as well as extensive numerical simulations of Thomson scattering, the theoretical foundations of a novel interaction geometry for laser-matter interaction are developed. This new method is very general and when tailored towards relativistically moving targets not being limited by the focusability (Rayleigh length) of the laser, while it does not require a waveguide. In a theoretical investigation of Thomson scattering, the optical analogue of undulator radiation, the limits of Thomson sources in scaling towards higher peak brilliances are highlighted. This leads to a novel method for generating brilliant, highly tunable X-ray sources, which is highly energy efficient by circumventing the laser Rayleigh limit through a novel traveling-wave Thomson scattering (TWTS) geometry. This new method suggests increases in X-ray photon yields of 2-3 orders of magnitudes using existing lasers and a way towards efficient, optical undulators to drive a free-electron laser. The results presented here extend far beyond the scope of this work. The possibility to use lasers as particle accelerators, as well as optical undulators, leads to very compact and energy efficient synchrotron sources. The resulting monoenergetic radiation of high brilliance in a range from extreme ultraviolet (EUV) to hard X-ray radiation is of fundamental importance for basic research, medical applications, material and life sciences and is going to significantly contribute to a new generation of radiation sources and free-electron lasers (FELs).