L'objectif de cette thèse était de développer un magnétomètre à force de Faraday pour mesurer des valeurs absolues de l'aimantation à très basse température (30 mK) et fort champ magnétique (16 T) avec une haute sensibilité (10-5 emu). Ce magnétomètre sera principalement utilisé pour sonder les propriétés induites sous champ dans les systèmes magnétiques frustrés.Dans une première partie, je détaille le développement de ce magnétomètre. Cela comprend l'optimisation du réfrigérateur à dilution et de bobines de gradient de champ ainsi que le développement d'une détection capacitive avec un étage amplificateur à froid pour améliorer la sensibilité de la mesure. Les mesures magnétiques préliminaires sont présentées. Les changements nécessaires pour rendre le magnétomètre opérationnel sont discutés.Dans une seconde partie, je présente l'étude expérimentale de systèmes magnétiques frustrés: des grenats de Gadolinium, décrits par des spins classiques, et des composés moléculaires frustrés à base de Cuivre, pour sonder les effets quantiques. Ces mesures ont été réalisées entre 70 mK et 300 K sur les magnétomètres existant à l'Institut Néel.Dans Gd3Ga5O12, nous avons complété le diagramme de phases H-T. Nous avons montré la robustesse de ce diagramme de phases par notre étude sur le composé isomorphe GGd3Al5O12. Nous avons mis en évidence la convergence de toutes les phases observées en un unique point dans les deux systèmes.Dans les systèmes quantiques, nous avons réalisé des études préliminaires sur des clusters Cu44 à base de tétraèdres, et un système triangulaire Cu3. Bien que prometteuses, nous n'avons pas approfondi ces études à cause de problèmes d'échantillons. / The objective of this work was to develop a Faraday force magnetometer to measureabsolute values of the magnetization at very low temperatures (30 mK) andhigh applied magnetic fields (16 T) with a high sensitivity (10-5 emu). This magnetometer will be especially dedicated to the study of the field induced properties of frustrated magnets.In a first part, I present the development of this magnetometer. It involves the optimization of the dilution refrigerator and field gradient coils, and the development of a capacitive detection with a cold amplifier stage to improve the measurement sensitivity. Preliminary magnetic measurements are shown. The changes in the design required to make the magnetometer operational are discussed.In a second part, I focus on experimental studies of frustrated magnets: Gadolinium garnets, described by classical spins, and Copper based frustrated molecular compounds, to probe quantum effects. These measurements were performed from 70 mK to 300 K, with the existing magnetometers at the Institut Neel.In Gd3Ga5O12, we have complemented the H-T phase diagram. This phase diagram was proven to be robust by our study on the isomorphous compound, Gd3Al5O12. We evidence the convergence of all the observed phases to a unique point in both samples.In quantum systems, we performed preliminary studies on Cu44 clusters with tetrahedral motives, and on a triangular system Cu3. Although promising, these studies were not pursued due to sample problems.

A eficácia de métodos convencionais de transmissão, utilizados para medir absorção de materiais altamente transparentes, é geralmente limitada pela reflexão e espalhamento de luz. A espectroscopia de Lente Térmica, por outro lado, não é sensível a esses fenômenos, e tem sido amplamente usada na determinação de baixas absorções ópticas. Neste trabalho, estudamos uma configuração de Lente Térmica de duplo feixe (onda contínua cw), desenvolvida recentemente, e suas aplicações. Essa configuração otimiza a técnica de Lente Térmica, e aumenta significativamente a sensibilidade de medida. Foram realizados alguns cálculos computacionais e testes experimentais dessa configuração, e os resultados foram comparados com os de outra configuração, tradicionalmente utilizada, denominada de feixe duplo no modo-descasado. Várias aplicações foram feitas para líquidos e sólidos. Como resultado, obtivemos o espectro de absorção da água pura entre 350 e 528 nm, que indicou um valor mínimo de aproximadamente 1,5 &#8226 10-5 cm-1 em torno de 380 nm, que é mais baixo do que todos os valores da literatura. Coeficientes tão baixos quanto 2 &#8226 10-7 cm-1 podem ser medidos para a água, com 1W de potência, utilizando essa configuração otimizada. Estimamos um limite de detecção de ~ 6 &#8226 10-9 cm-1 (P = 1 W) para o solvente CCl4, que corresponde (até onde sabemos) ao menor valor já encontrado na literatura para líquidos, utilizando-se laser cw. Quanto à detecção de traços de impurezas, o limite para o Cr (III) em solução aquosa foi de ~ 40 ppb (ng/mL) em 514 nm, que corresponde a aproximadamente metade da concentração máxima ideal de Cr (III) em águas potáveis e naturais. Foram obtidos alguns resultados preliminares para a variação do caminho óptico com a temperatura (ds/dT), em sólidos com diferentes geometrias. Para a sílica fundida (quartzo vítreo) Suprasil, determinamos um limite superior para o coeficiente de absorção, cujos valores, 1 &#8226 10-6 cm-1 (em 493 nm) e 1 &#8226 10-5 cm-1 (em 355 nm), também são menores do que os resultados da literatura nessa região do espectro. A alta sensibilidade da técnica permitiu obter a absorção, em 1064 nm, das matrizes de materiais laser dopados com Nd3+, sendo (1,8 &#177 0,1) &#8226 10-3 cm-1 para o vidro Q-98 (Kigre), e (5 &#177 1 &#8226 10-4 cm-1 para o cristal Nd:YAG. Realizamos também medidas de eficiência quântica de fluorescência em nanocristais semicondutores (CdSe/ZnS) suspensos em THF e tolueno, com resultado aproximadamente 5 vezes mais preciso do que o obtido por técnica convencional de fluorescência. As principais vantagens da configuração otimizada, em relação à tradicional, são: um procedimento experimental simples, boa precisão nas medidas de difusividade térmica e, principalmente, a alta sensibilidade da técnica. As desvantagens são: um tempo de medida mais longo, e a necessidade de amostras maiores. / The efficiency of conventional transmission methods used to measure absorption of hightransparent materials is usually limited by light scattering and reflection. On the other hand, Thermal Lens spectroscopy is insensible to such phenomena and has been widely applied to determinate low optical absorptions. In this thesis, we have studied a recently developed dualbeam (continuous wave - cw) Thermal Lens configuration as well as its practical applications. This configuration optimizes the technique and significantly improves the measurement sensitivity. Some computational calculations and experimental tests of this approach were carried out. The results were compared with those obtained using a traditional configuration, named Mode-mismatched Dual-beam Thermal Lens. Several applications were made for liquids and solids. As a result, we obtained the absorption spectrum for pure water in the range of 350 to 528 nm, which indicated a minimal value of approximately 1,5 &#8226 10-5 cm-1 around 380 nm, that is lower than those found in literature. Absorption coefficients as small as 2 &#8226 10-7 cm-1, can be measured for water, using 1W of excitation power, with this optimized configuration. We have estimated a detection limit of ~ 6 &#8226 10-9 cm-1 (P = 1 W) for CCl4 solvent, which corresponds (to the best of our knowledge) to the smallest value found in the literature for liquids using cw laser. With regard to the chemical trace analysis, the detection limit was ~ 40 ppb (ng/mL) at 514 nm for Cr (III) in aqueous solutions, which is nearly half of the maximum desired Cr (III) concentration in drinking and natural waters. Some preliminary results for the temperature coefficient of the optical path length (ds/dT) were obtained at solids with different geometries. For the fused-silica (vitreous quartz) Suprasil, we have determined an upper limit for the absorption coefficient, whose values, 1 &#8226 10-6 cm-1 at 493 nm, and 1 &#8226 10-5 cm-1 at 355 nm, also are lower than the values found in literature in this spectrum region. The high sensitivity of the technique allowed us to measure the absorption (at 1064 nm) of matrices of Nd3+ doped laser materials: (1,8 &#177 0,1) &#8226 10-3 cm-1 for Q-98 glass (Kigre), and (5 &#177 1) &#8226 10-4 cm-1 for Nd:YAG crystal. We carried out as well measurements of fluorescence quantum yield of semiconductor nanocrystals (CdSe/ZnS) suspended in THF and toluene solvents, whose result was approximately 5 times more accurate than that obtained with the conventional fluorescence technique. The main advantages of the optimized configuration are: a simple experimental procedure, a good accuracy for thermal diffusivity measurements, and most important the high sensitivity of the technique. The drawbacks are: a longer time of measurements, and the requirement of larger samples.

(1) Background: Patients with severe chronic kidney disease (CKD G4–G5) often have chronically elevated high-sensitivity cardiac troponin T (hs-cTnT) values above the 99th percentile of the upper reference limit. In these patients, optimal cutoff levels for diagnosing non-ST-elevation acute coronary syndrome (NSTE-ACS) requiring revascularization remain undefined. (2) Methods: Of 11,912 patients undergoing coronary angiography from 2012 to 2017 for suspected NSTE-ACS, 325 (3%) had severe CKD. Of these, 290 with available serial hs-cTnT measurements were included, and 300 matched patients with normal renal function were selected as a control cohort. (3) Results: In the CKD cohort, 222 patients (76%) had NSTE-ACS with indication for coronary revascularization. Diagnostic performance was high at presentation and similar to that of the control population (AUC, 95% CI: 0.81, 0.75–0.87 versus 0.85, 0.80–0.89, p = 0.68), and the ROC-derived cutoff value was 4 times higher compared to the conventional 99th percentile. Combining the ROC-derived cutoff levels for hs-cTnT at presentation and absolute 3 h changes, sensitivity increased to 98%, and PPV and NPV improved up to 93% and 86%, respectively. (4) Conclusions: In patients with severe CKD and suspected ACS, the diagnostic accuracy of hs-cTnT for the diagnosis of NSTE-ACS requiring revascularization is improved by using higher assay-specific cutoff levels combined with early absolute changes.

[pt] Esta dissertação tem por objetivo o desenvolvimento de um transdutor de pressão de alta sensibilidade, baseado nas características de fase da impedância de sensores de Magnetoimpedância Gigante. A configuração do dispositivo visa a aplicações biomédicas, tais como medições da onda de pulso arterial e de sua velocidade de propagação. Projetou-se um sistema de transdução de pressão em tensão, que contém um módulo intermediário baseado em um magnetômetro GMI. O protótipo implementado inclui uma estrutura mecânica, responsável pela transdução de pressão em campo magnético, e um circuito eletrônico, responsável pela conversão deste em uma tensão elétrica de saída. A conversão de pressão em campo magnético é feita por meio de uma fonte de campo magnético aderida a uma membrana elástica. Foram realizados estudos comparativos empregando agulhas magnetizadas e ímãs permanentes como fontes móveis de campo. Por sua vez, o elemento sensor GMI utilizado foi experimentalmente caracterizado, a fim de se obter suas curvas características de módulo e fase, em função do campo magnético. O circuito eletrônico de transdução foi projetado e avaliado de forma computacional e experimental. As principais características do mesmo são detalhadas ao longo do texto e as previsões teórico-computacionais são comparadas com os resultados experimentais obtidos. Por sua vez, parâmetros chave do protótipo desenvolvido são minuciosamente analisados, tais como: sensibilidade, linearidade e resposta em frequência. Também, avalia-se a densidade espectral de ruído do transdutor desenvolvido e estima-se sua resolução na banda de passagem. Os resultados obtidos indicam que o protótipo de baixo custo desenvolvido apresenta alta resolução e alta sensibilidade, além de uma banda de passagem compatível com a requerida pelas aplicações biomédicas nas quais deseja-se empregá-lo. Dessa forma, espera-se que o dispositivo desenvolvido contribua para o avanço tecnológico do ferramental utilizado no setor da saúde. / [en] This dissertation aims at the development of a high sensitivity pressure transducer, based on the phase impedance characteristics of Giant Magnetoimpedance sensors. The configuration is intended to employ the developed device in biomedical applications, such as in measurements of arterial pulse wave and pulse wave velocity. A transduction system of pressure into voltage was designed, which contains an intermediate module based on a GMI magnetometer. The idealized prototype contains a mechanical structure, responsible for converting pressure into magnetic field, and an electronic circuit, responsible for converting the latter into a voltage output. The conversion of pressure into magnetic field is performed by means of a magnetic field source adhered to an elastic membrane. Comparative studies were carried out using magnetized needles and permanent magnets as field sources. In turn, the GMI sensor element was experimentally characterized in order to evaluate how its impedance magnitude and phase are affected by the magnetic field. The influence of the cable length used to interconnect the GMI sensor to the electronic circuit is also discussed. The electronic transduction circuit was designed and analyzed by computational and experimental evaluations. The main features of the circuit are detailed throughout the text and the theoretical and computational predictions are compared with the obtained experimental results. Furthermore, the key parameters of the developed prototype are meticulously analyzed, such as: sensitivity, linearity and frequency response. Also, the spectral noise density of the developed transducer is evaluated and its resolution in the passband is estimated. The obtained results indicate that the developed prototype presents low cost of manufacture and operation, high resolution, high sensitivity and a passband compatible with the requirements imposed by the biomedical applications of interest. In this way, it is intended that the device developed in the present Dissertation contributes to the technological enhancement of measurement equipment used in health sector.

[pt] Esta Tese teve por objetivo desenvolver um magnetômetro de alta sensibilidade, baseado nas características de fase do efeito da Magnetoimpedância Gigante (GMI – Giant Magnetoimpedance), para medição de campos magnéticos ultra-fracos. Elementos sensores GMI apresentam grande potencial na fabricação de magnetômetros que conciliem alta sensibilidade e elevada resolução espacial com baixo custo. A otimização da sensibilidade do transdutor magnético é diretamente afetada pela sensibilidade de seus elementos sensores GMI, cuja maximização é um processo intrinsecamente multivariável. Consequentemente, a metodologia experimental empregada iniciou-se pelo desenvolvimento de um sistema automático de caracterização das amostras GMI, de modo a se garantir a agilidade do processo de caracterização, possibilitando a obtenção de um volume significativo de informações experimentais. A análise minuciosa dos dados provenientes das medições experimentais permitiu a definição do ponto ótimo de operação das amostras GMI estudadas. Em todas as medições experimentais realizadas foram obtidas e avaliadas as curvas de histerese das amostras GMI. Na sequência, foram idealizados circuitos eletrônicos para condicionamento das amostras GMI e leitura das características de fase de sua impedância, destacandose a configuração eletrônica desenvolvida para a amplificação da sensibilidade de fase. Foram, inclusive, depositadas patentes nacionais e internacionais referentes ao método proposto e ao novo transdutor magnético GMI (PI 0902770-0; PI 1004686-0; WO/2010/094096 e WO/2012/048395). As caracterizações e ensaios experimentais realizados indicaram a eficácia da abordagem proposta, evidenciando o grande potencial do magnetômetro GMI desenvolvido, o qual apresentou uma elevada sensibilidade de 5 mV/nT. A resolução do magnetômetro foi limitada pelo ruído magnético ambiental, indicando que sua capacidade de medição de campos inferiores aos níveis de ruído poderá ser claramente evidenciada quando for avaliada em ambiente magneticamente blindado. Os estudos teórico-experimentais realizados indicam o potencial do transdutor magnético GMI desenvolvido, caracterizado por seu baixo custo e elevada sensibilidade, para aplicação na medição de campos magnéticos ultra-fracos. / [en] This Thesis aimed at developing a high sensitivity magnetometer, based on the phase characteristics of the Giant Magnetoimpedance effect (GMI), for measuring ultra-weak magnetic fields. GMI sensor elements have great potential to implement magnetometers that combine high sensitivity and high spatial resolution with low cost. The optimization of the magnetic transducer sensitivity is directly affected by the sensitivity of its GMI sensor elements, whose maximization is inherently multivariate. Consequently, the first step of the experimental methodology employed was to develop an automatic system for the characterization of GMI samples, so as to ensure the agility of the characterization process, allowing the gathering of a significant amount of experimental data. A thorough analysis of the experimental data led to the definition of the optimal operation point of the analyzed GMI samples. The hysteresis curves of the GMI samples were obtained and evaluated, in all of the performed experimental measurements. Based on the characterization studies results, electronic circuits were designed for conditioning the GMI samples and reading their impedance phase characteristics, highlighting the new electronic configuration developed for enhancing the phase sensitivity. National and international patents were filed, related to the proposed method, for sensitivity enhancement, and to the new GMI magnetometer (PI 0902770-0; PI 1004686-0; WO/2010/094096 e WO/2012/048395). The performed experimental characterizations and assays indicated the effectiveness of the proposed approach, showing the great potential of the developed GMI magnetometer, which presents a high sensitivity of 5 mV/nT. The magnetometer resolution was limited by the environmental magnetic noise, pointing out their capability in measuring fields below the environmental noise level, which can be clearly evidenced only when evaluated in a magnetically shielded room. The theoretical and experimental studies carried out indicate the potential of the developed GMI magnetic transducer, characterized by its low cost and high sensitivity, for applications involving the measurement of ultra-weak magnetic fields.

[pt] Esta Tese tem por objetivo o desenvolvimento de um sistema destinado à medição de campo magnético com alta sensibilidade e resolução, baseado nas características de fase da impedância em sensores que apresentam o efeito GMI, e a otimização das características de desempenho por meio do uso de configurações em malha fechada. A metodologia empregada inicia com a avaliação experimental das características de fase da impedância de amostras de diferente estrutura e composição química, em função do campo magnético externo, a fim de selecionar aquelas com alta sensibilidade, baixa histerese e maior homogeneidade. Na sequência, são realizadas avaliações teórico-computacionais dos transdutores magnéticos em malha aberta e fechada (magnetômetro e gradiômetro). Da mesma forma, as principais características dos circuitos e controladores software dos transdutores desenvolvidos são detalhadas ao longo do texto. Por sua vez, as principais figuras de mérito dos protótipos desenvolvidos são detalhadamente analisadas, tais como: sensibilidade, linearidade, resposta em frequência, densidade espectral de ruído e resolução. As caracterizações e ensaios experimentais realizados evidenciaram o grande potencial dos transdutores GMI em malha fechada para a atenuação da interferência 1/f, aprimoramento da linearidade e ampliação da faixa de operação. O magnetômetro GMI em malha fechada apresentou sensibilidade em torno de 75,8 mV/microteslas, fundo de escala maior que mais ou menos 40 microteslas, banda de passagem de 45 Hz e resolução na banda de passagem de 27,74 nT. Por outro lado, o gradiômetro GMI em malha fechada desenvolvido apresentou sensibilidade em torno de 102 mV/microteslas, fundo de escala maior que mais ou menos 40 microteslas, banda de passagem de 30 Hz e resolução na banda de passagem de 28,41 nT. / [en] This Thesis aims to develop a system for magnetic field measurement with high sensitivity and resolution, based on the impedance phase characteristics of sensors that have the GMI effect and the performance characteristics optimization through closed-loop configurations. The methodology starts with the experimental evaluation of the phase characteristics of the impedance in samples of different chemical composition and structure as a function of the external magnetic field in order to select those with high sensitivity, low hysteresis, and higher homogeneity. Subsequently, theoretical-computational assessments of magnetic transducers in open and closed-loop (magnetometer and gradiometer) are carried out. Likewise, the main characteristics of the circuits and software controllers of the developed transducers are detailed throughout the text. In turn, the main figures of merit of the developed prototypes are analyzed in detail, such as sensitivity, linearity, frequency response, noise spectral density, and resolution. The characterizations and experimental tests carried out showed the great potential of GMI transducers in a closed-loop configuration for attenuation of interference 1/f, improving linearity and expanding the operating range. The closed-loop GMI magnetometer showed a sensitivity of around 75.8 mV/microteslas, a full-scale range greater than plus or minus 40 microteslas, a pass band of 45 Hz and a resolution in the pass band of 27.74 nT. On the other hand, the GMI closed-loop gradiometer developed had a sensitivity of around 102 mV/microteslas, a full scale greater than plus or minus 40 microteslas, a passband of 30 Hz and a resolution in the pass band of 28.41 nT.

Our study provided an analysis and comparison of specific blood values, dietary intake, body composition, and inflammatory markers (high sensitivity-C-reactive protein (HS-CRP), tumor necrosis factor-alpha (TNF-α), and interleukin-6 (IL-6)) between adults with type 2 diabetes mellitus (T2DM) and prediabetes (PDM) to adults without diabetes. A total of 22 participants (PDM/T2DM n=12, controls n=10) in the San Luis Obispo, CA area completed the study prior to our ending recruitment due to Covid-19. Body composition data were collected through DXA scans. Dietary intake was assessed using a 3-day food record survey and nutritional analysis conducted using ESHA food processing software. In addition, participants completed an overnight fast and early morning blood draw for evaluation of blood glucose regulation, blood lipid profile and inflammatory biomarkers. Analysis included a series of randomization tests that were conducted to determine possible statistical differences between the mean of basic characteristics (age, BMI, weight, HbA1C, fasting plasma glucose, fasting insulin, triglycerides, LDL, HDL, and total cholesterol levels) of the control group and the PDM/T2DM group. Secondly, 2-way ANOVA statistical analyses were conducted to determine the interaction between sex and diabetes status on caloric intake, macronutrient distribution, quality of fat intake, visceral adipose tissue (VAT), and inflammatory biomarkers. We found there was a significant difference in fasting plasma glucose (FPG) and hemoglobin A1C (HbA1C) between the control group and the PDM/T2DM group. We did not find a statistically significant difference in caloric intake, macronutrient distribution, quality of fat intake, visceral adipose tissue (VAT), and inflammatory biomarkers between the PDM/T2DM and control group. Due to the lack of studies that include adults with PDM, we concluded additional future research needs to focus on blood biochemistry values, dietary intake, body composition, and inflammatory markers health-risk factors in both adults with PDM and T2DM since these values can improve diagnosis and treatment of T2DM.

Immunoassays are analytical methods that use the highly specific binding of antibodies in order to detect and quantify an analyte. The technique has become a staple in modern biopharmaceutical research and diagnostics, however the measurement of biomarkers like dysregulated cytokines require ultra-sensitive immunoassays that can detect molecules at sub pg/mL concentrations. One such method is the Exazym® signal amplification. Based on a method called Binding Oligo Ladder Detection (BOLD), it is a set of add-on reagents where a primer is conjugated to a detection antibody which is then combined with a template, polymerase and modified DNA nucleotides to generate a oligonucleotide ladder that is detected with a secondary detection antibody; this amplifies the signal by a factor of 10-100 in an existing immunoassay.  By applying this method to the Gyrolab® microfluidic immunoassay system, a sensitivity increase of 880x-1800x was achieved between a pre-synthesised BOLD product and the polymerised BOLD product. Several key factors for successful polymerisation in the microfluidic system were identified: adding the template separately before the polymerase and using a buffer with low ionic strength for the secondary detection antibody. Applying the BOLD amplification to an existing Gyrolab TNF-α assay only resulted in similar sensitivity as previous methods however. This report demonstrates that BOLD amplification can be successfully performed in a flow-through format on miniaturized affinity columns in the Gyrolab system to increase the sensitivity by orders of magnitude, where both the immunoassay and the amplification steps are automated in the system. However, further optimisation is needed for application in biomarker assays.

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.