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1
Peter, F. "Advanced emitters and detectors for terahertz time-domain spectroscopy." Forschungszentrum Dresden, 2010. http://nbn-resolving.de/urn:nbn:de:bsz:d120-qucosa-61479.
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The idea of terahertz-time-domain spectroscopy (THz-TDS) is to exploit a single cycle, spectrally broad THz radiation pulse to gain insight into the response of matter. Photoconductive devices and nonlinear crystals are utilized in both the generation as well as the coherent detection of THz radiation. The relatively high cost and the complexity of commonly used titanium-sapphire lasers hinder a more widespread use of pulsed THz systems for commercial applications. Er-doped femtosecond fiber lasers operating at 1.55 μm could offer a viable alternative. In this thesis nonlinear crystals and photoconductive emitters are discussed for excitation in the near infrared (NIR) window of between 800 nm to 1550 nm. The main focus of this thesis is a detailed study of substrate materials for an interdigitated photoconductive antenna. Photoconductive antennas with microstructured electrodes provide high electric acceleration fields at moderate voltages because of small electrode separations. The scalability of these devices allows for large active areas in the mm^2 range, which are sufficient for excitation at large optical powers. In comparison with conventional emitter structures, these antennas have more favourable characteristics regarding THz power, spectral properties, and ease of handling. Depending on the utilized substrate material, photoconductive antennas can then be operated using different excitation wavelengths. By employing substrates with short carrier trapping times these antennas can be operated as THz-detectors. Moreover the design of electrode structures for generating radially and azimuthally polarized THz waves are presented. A second topic deals with the signal analysis and signal interpretation of THz pulses transmitted through several material systems. These experiments show the potential for tomographic and spectroscopic applications. The third part deals with THz emission by frequency mixing in nonlinear organic and inorganic crystals. Hereby the focus is on polaritonic phase matching in GaAs. Furthermore, indications of THz tunability by the excitation wavelength were found by utilizing waveguide structures. However, the observed tuning range is much lower then theoretically predicted. Specific reasons for this are discussed.
2
Rasekh, Payman. "Kerr Effect at the THz Frequencies." Thesis, Université d'Ottawa / University of Ottawa, 2020. http://hdl.handle.net/10393/41085.
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This doctoral dissertation focuses on the nonlinear optical response of water vapour as well as some solids at terahertz (THz) frequencies. In this study, the propagation of broadband single-cycle THz pulses through a medium with the third-order nonlinear optical response is theoretically investigated. Also, a technique to measure the nonlinear response of transparent materials based on the time-domain THz spectroscopy is developed, which provides frequency dispersion curves of the nonlinear Kerr coefficient (n₂).
A numerical model is used to simulate the THz pulse propagation. This model takes
into account non-paraxial effects, self-focusing, and diffraction, as well as dispersion,
in both the linear and nonlinear optical regimes. The contribution of non-instantaneous
Kerr-type nonlinearity to the overall instantaneous and delayed Kerr effect at the THz
frequencies is investigated. It is shown how increasing the nonlinear relaxation time and its dispersion modifies the THz pulse after the propagation through a transparent medium. The effect of linear dispersion on self-action during pulse propagation is also discussed.
Moreover, the nonlinear spectroscopy of water vapour at THz frequencies is reported. Atmospheric water vapour has a rich spectrum with several strong resonances at frequencies below 3 THz, falling within the range of operation of most existing THz sources. An extremely large nonlinear response to THz radiation is observed at the positions of these resonances. Using the optical Kerr model for the nonlinear response, a minimum nonlinear refractive index of the order of 10² m²/W is estimated. The results provide insight into the energy levels of the water molecule and give a more accurate picture of its response to electromagnetic radiation, paving the way to more accurate THz spectroscopy, imaging, and sensing systems, and thereby facilitating future emerging THz technologies.
Finally, the nonlinear response of solids at THz frequencies is studied. It has been
shown that a phonon-induced THz Kerr effect can result in a larger nonlinear refractive
index than the nonlinear refractive index at the visible or near-infrared range (optical
Kerr effect). This pronounced nonlinear optical behavior is verified using a time-domain characterization approach. The results indicate a large delay occurred to the THz fields as they transmit through some of the material samples. In the frequency domain, the induced nonlinear phase shift of the intense THz field is shown to be relatively large of the order of 0.1 rad. From the phase information, the nonlinear phase is extracted by which the dispersion profile of n₂ is obtained.
3
Bernerd, Cyril. "Génération d'ondes TeraHertz par Différence de Fréquence." Thesis, Université Grenoble Alpes (ComUE), 2018. http://www.theses.fr/2018GREAT061/document.
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Le domaine des ondes TeraHertz (THz) s’étend de l’infrarouge lointain (15 μm / 20 THz) aux ondes radios (3000 μm / 0.1 THz). La couverture spectrale des sources actuelles, qu’elles soient thermique (lampes à mercure…), électronique (diode Gunn…) ou optique (laser, antennes…), ne permet pas de répondre à l’ensemble des applications en spectroscopie et en imagerie. Une alternative à ces sources est l’optique non linéaire paramétrique, qui permet de générer des ondes THz à partir du processus de Différence de Fréquences (DFG), et qui consiste à injecter un ou deux lasers dans un cristal non linéaire. Afin de couvrir au mieux le très large domaine THz, il est nécessaire de déterminer un ensemble de cristaux dont les propriétés optiques permettent de générer ces ondes avec de forts rendements de conversion.Le travail présenté dans ce manuscrit de thèse décrit l’étude de ces propriétés pour un ensemble de cristaux non linéaires, ainsi que des résultats expérimentaux de génération THz à partir de la DFG entre deux lasers monochromatiques en régime nanoseconde et picoseconde, ou entre deux composantes de Fourier au sein d’une impulsion laser femtoseconde. Nous avons sélectionné vingt nouveaux cristaux jamais étudiés dans le domaine THz auparavant, ainsi que le nouveau cristal organique de BNA. Nous avons mesuré leurs spectres de transmission du visible au THz, ainsi que les propriétés optiques non linéaires incluant les conditions d’accord de phase et le rendement de conversion<br>THz-waves extend from the far InfraRed (15 μm – 20 THz) to radio waves (3000 μm – 0.1 THz). Current sources based on thermal (Mercury lamps…), electronics (Gunn diode...) or optics (laser, antennas…) technologies can’t cover this wide spectral range for applications in spectroscopy and imaging. An alternative is provided by parametric nonlinear optics, which leads to the generation of THz waves from Difference Frequency Generation (DFG) by injecting one or two lasers in a nonlinear crystal. To better cover the wide THz domain, it is necessary to determine nonlinear crystals with optical properties leading to the generation of such waves with high conversion efficiencies.This PhD thesis is devoted to the study of these properties for a panel of nonlinear crystals, along with experimental results of THz generation from DFG between two monochromatic lasers in the nanosecond and picosecond regimes, or between two Fourier components within a femtosecond laser. We selected twenty new crystals never studied before in the THz domain, along with the organic crystal of BNA. We measured their transmission spectra from visible to THz, and their nonlinear properties including phase-matching conditions and conversion efficiency
4
Nguyen, Alisée. "Contrôle de rayonnements térahertz intenses produits par lasers femtosecondes et applications à la détection de molécules." Thesis, Université Paris-Saclay (ComUE), 2019. http://www.theses.fr/2019SACLS020/document.
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Les ondes térahertz (THz), situées entre l'infrarouge et les micro-ondes dans le spectre électromagnétique, correspondent aux fréquences caractéristiques de nombreux mouvements moléculaires et permettent ainsi de caractériser des molécules complexes par spectroscopie dans le domaine temporel. Cette thèse a pour objectif d'étudier les champs THz émis par une source constituée d'une impulsion laser à deux couleurs générant un plasma par ionisation de l'air. En raison de l'asymétrie temporelle du champ laser, un courant électronique présentant une composante basse-fréquence dans la gamme THz est formé dans le plasma par conversion non linéaire et produit un champ secondaire comprenant une composante THz. Les effets non linéaires intervenant dans la génération du rayonnement THz sont l'effet Kerr à basse intensité (< 10¹³ W/cm²) et les photocourants à plus haute intensité (> 10¹³ W/cm²), au-dessus du seuil d'ionisation. Ce dernier mécanisme, qui génère le plus de rayonnement THz, est principalement étudié dans ce manuscrit. Si la puissance crête de l'impulsion laser est suffisamment élevée, des filaments de lumière peuvent être formés par combinaison de l'effet Kerr focalisant et de la formation d'un plasma défocalisant. Le phénomène de filamentation laser permet ainsi de créer des ondes THz à distance. En modulant l'impulsion laser, il est aussi possible de modifier les champs et spectres THz associés. En particulier, nous étudions les effets d'une dérive de fréquence et de la combinaison de multi-impulsions sur l'efficacité de conversion laser-THz. Nous consacrons en outre une large part de nos études à l'influence de l'augmentation de la longueur d'onde laser sur le rendement en énergie de l'émission THz<br>The terahertz waves (THz), located between the infrared and the microwaves in the electromagnetic spectrum, correspond to the characteristic frequencies of numerous molecular motions and thus make it possible to characterize complex molecules by time-domain spectroscopy. This thesis aims to study the THz fields emitted by a source formed by a two-color laser pulse generating a plasma by air ionization. Due to the time asymmetry of the laser field, an electric current having a low-frequency component in the THz range is formed in the plasma by nonlinear conversion, generating a secondary field including a THz component. The nonlinear effects involved in the generation of THz radiation are the Kerr effect at low intensity (< 10¹³ W/cm²) and the photocurrents at higher intensity (> 10¹³ W/cm²), above the ionization threshold. This latter mechanism, which generates the most THz radiation, is mainly studied in this manuscript. If the peak power of the laser pulse is sufficiently high, light filaments can be created by combining the focusing Kerr effect and the defocusing action of the plasma. So, the filamentation process can produce THz waves remotely. By modulating the laser pulse, it is possible to modify the associated THz fields and spectra. In particular, we study the effects of pulse chirping and multi-pulse combination. We also devote a large part of our studies to the influence of increasing the laser wavelength on the THz energy yield
5
Singh, Rohit. "Modulated orientation sensitive terahertz spectroscopy." Thesis, State University of New York at Buffalo, 2013. http://pqdtopen.proquest.com/#viewpdf?dispub=3565883.
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<p> The energies of protein correlated motions lie in the far infrared or THz frequency range (λ = 1 cm – 50 mm, f = 0.03 – 6 THz). The existence of correlated motions has been confirmed by neutron and inelastic x-ray scattering measurements. These techniques require large sample volumes and specialized facilities, limiting their application to systematic studies of changes in correlated motions with functional state and allosteric interactions. Standard terahertz time domain spectroscopy measurements have shown sensitivity to protein-ligand binding, oxidation state, conformation, temperature and hydration. However, the response is broad, in part from the large vibrational density of states and in part from the dielectric response contribution from surface water and side-chains. </p><p> As an overall strategy to measure the correlated structural motions in protein, we use anisotropic and birefringent behavior of molecular crystals to develop a new technique called MOSTS (Modulated Orientation Sensitive Terahertz Spectroscopy). We achieve high sensitivity and mode separation, by using single molecular crystal such as sucrose and oxalic acid, and rapid modulation of the relative alignment of the terahertz polarization and the crystal axes by rotating the sample. By locking into the signal at the rotation frequency, we determine the polarization sensitive signal and map out the optically active vibrational resonances. To illustrate the technique, we compare our measured spectra with the calculated, and find a close agreement. </p><p> We measure dielectric properties of oxalic acid, sucrose and protein crystals and polycarbonate sheet using standard terahertz time domain spectroscopy. We determine the absorbances in oxalic acid and sucrose crystals, using MOSTS technique. We compare the resonances in these two distinct methods. Then, we develop a protein model sample by sticking together two thin plates of sucrose and polycarbonate. We carry out standard THz-TDS and MOSTS measurements on the protein model sample. We show that we are able to isolate the vibrational modes from glassy background in protein model sample by using MOSTS.</p>
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Brandt, Nathaniel Curran. "Developments and advances in nonlinear terahertz spectroscopy." Thesis, Massachusetts Institute of Technology, 2014. http://hdl.handle.net/1721.1/91110.
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Thesis: Ph. D., Massachusetts Institute of Technology, Department of Chemistry, 2014.<br>Cataloged from PDF version of thesis.<br>Includes bibliographical references.<br>Nonlinear terahertz (THz) spectroscopy is a rapidly developing field, which is concerned with driving and observing nonlinear material responses in the THz range of the electromagnetic spectrum. In this thesis, I present several advances in nonlinear THz spectroscopy that expand the range of systems in which responses may be driven, the types of responses that may be initiated, and the way in which these responses may be observed. Sufficiently strong THz pulses are generated using the tilted-pulse-front technique, and are collected, focused, and detected using a THz spectrometer specifically designed for maximum peak THz electric field strength and maximum flexibility, allowing for a wide range of experimental geometries to be implemented. Further enhancement in the peak THz electric field strength is obtained through the use of metamaterial structures, which concentrate free-space THz fields in their antenna gaps. Impact ionization was observed in high-resistivity silicon, a material in which no nonlinear THz response had been previously seen, using metamaterial structures to enhance free space THz electric fields. Using three-dimensional metamaterial structures, the THz magnetic field is shown to also be capable of driving ionization processes both in high-resistivity silicon as well as air. Using metamaterial structures with open gaps, the THz electric field is shown to induce breakdown in air at both high and low pressures due to field ionization processes involving the gold metamaterial antennas. Furthermore, THz-driven electromigration of the gold metamaterial antennas is observed. Probing of THz-driven structural changes in both vanadium dioxide and perovskite ferroelectrics is demonstrated using femtosecond Xray pulses from the LCLS facility at the SLAC National Accelerator Laboratory. Finally, ongoing results involving energetic materials, stimulated Raman measurements, and Stark effect measurements are discussed. This work, coupled with the ongoing expansion of nonlinear THz techniques and potential applications demonstrates the continued development of nonlinear THz spectroscopy into a robust and valuable method for investigating fundamental processes in a multitude of systems.<br>by Nathaniel Curran Brandt.<br>Ph. D.
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Kühn, Wilhelm. "Nonlinear terahertz spectroscopy in one and two dimensions." Doctoral thesis, Humboldt-Universität zu Berlin, Mathematisch-Naturwissenschaftliche Fakultät I, 2011. http://dx.doi.org/10.18452/16286.
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Die vorliegende Dissertation behandelt Grundlagen und Anwendungen der nichtlinearen Terahertzspektrospie (THz). Diese Arbeit zeigt erstmalig, dass sich die Inversion des Quantenkaskadenlasers nach einer Störung schon innerhalb von hundert Femtosekunden wieder erholt. Außerdem wurde der exakte Generationsprozess von THz Impulsen in einem Laser-induzierten zwei-Farben Plasma untersucht. Durch Vergleich mit Simulationen wird eindeutig der Ionisationsstrom im Plasma als Quelle der THz Strahlung identifiziert. Neue Spektroskopiemethoden in ein und zwei Zeitdimensionen werden entwickelt und auf verschiedene Halbleiterstrukturen angewendet. So wird das elektrische Feld des THz-Impulses für Hochfeld-Transportexperimente genutzt. Im quanten-kinetischen Regime entkoppelt die Elektronbewegung von den Phononmoden des Kristalls, und quasi-ballistischer Transport wird möglich. Wir entwickeln ein dynamisches Polaronmodell, welches sowohl die experimentellen Ergebnisse auf kurzen Zeitskalen als auch Literaturwerte auf langen Zeitskalen zuverlässig reproduziert. Bei niedrigen Temperaturen von 80 K tritt zusätzlich THz-induziertes Interbandtunneln in GaAs auf. Die temperaturabhängige Tunnelrate hängt dabei wesentlich von der Dekohärenzrate des induzierten Prozesses ab. Desweiteren wird eine kollineare 2D THz Spektroskopiemethode entwickelt und erstmals an Quantentrogstrukturen angewendet. Eine komplizierte, nichtkollineare Strahlgeometrie ist prinzipiell nicht notwendig. Die eingeführten Frequenzvektoren erklären das zugrundeliegende N-Wellen Mischen analog zum Raum auch in der Zeit. So werden mit einer kollinearen Strahlgeometrie alle nichtlinearen Signale simultan gemessen werden. Mit diesem Konzept wurden Rabi-Oszillationen an Intersubbandübergängen in Signale verschiedener nichtlinearer Ordnung zerlegt. Die ersten 2D Korrelationsspektren im THz-Bereich demonstrieren die energetischen Kopplungen zwischen verschiedenen polaronischen Zuständen in einer Doppel-Quantentrogstruktur.<br>The presented thesis concerns fundamentals and applications of nonlinear terahertz (THz) spectroscopy. It is demonstrates that the a gain recovery time of a quantum cascade laser (QCL) amounts only to several hundred femtoseconds. We explored the generation process of THz pulses within a laser-induced two-color plasma and identified the ionisation current as the origin of the THz radiation. Novel methods of THz spectroscopy in one and in two dimensions are developed and applied to different semiconductor heterostructures. We use the electric field of THz pulses for high-field transport experiments. Within this quantum-kinetic regime, the electron velocity decouples from phonon modes of the crystal lattice and quasi-ballistic transport becomes feasible during the first hundreds of femtoseconds. We develop a dynamic polaron model, which reproduces the experimental results on short time scales as well as the published values on long time scales. At low temperatures of 80 K, we find additional THz-induced interband tunneling in GaAs. The temperature dependent tunneling rate depends essentially on the decoherence time of the induced process. Furthermore, a novel method of collinear 2D THz spectroscopy is developed and applied to quantum well structures. Frequency vectors are introduced to explain the underlying process of N-wave mixing not in space, but in time. This allows for a collinear beam geometry to measure all nonlinear signals simultaneously. We used this new method to decompose Rabi oscillations on intersubband transitions into nonlinear signals of different order. The first 2D correlation spectra in the THz frequency range demonstrate energetic couplings between polaronic states within an asymmetric double quantum well structure. Another experiment displays for the first time the 2D correlation spectrum of a 2pi Rabi flop on the intersubband transition of a multiple quantum well structure.
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Ould-Hamouda, Amine. "Étude des transitions de phase photo-induites dans des matériaux métalliques et organométalliques." Thesis, Bordeaux, 2016. http://www.theses.fr/2016BORD0112/document.
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Ces travaux de thèse portent sur l'étude des transitions de phases photo-induites dans différents matériaux métalliques et organométalliques. Les études présentées ont été guidées par la problématique liée à l'enregistrement et au stockage d'informations numériques. Tout d’abord, nous nous sommes intéressés à la spectroscopie THz et Raman de composés à transitions d'état de spin à base de Fe (II). Les spectres obtenus à l’aide de ces deux techniques sont confrontés aux résultats issus de simulations numériques (DFT). Nous avons également étudié la transition d’état de spin induite par des lasers CO2 dans des composés à transition de spin polymériques. Un dispositif expérimental simple permettant l'enregistrement d'information dans ce type de matériaux est proposé. Par la suite, nous avons étudié la transition réversible de la phase métallique (λ métastable à semiconductricer (β stable) dans des nanoparticules d'un oxyde de Titane (Ti3O5), soumis à des impulsions laser nanosecondes. Nous avons étudié plus particulièrement les aspects cinétiques de cette transition. Il apparaît alors que la transition λ→β se produit sur une échelle de plusieurs centaines de nanosecondes, tandis que la transition β→λ se fait en quelques dizaines de nanosecondes. Les mécanismes photoythermiques à l’origine de cette transition permettent de rendre compte de ces observations expérimentales. Enfin, nous avons étudié un complexe bimétallique analogue du bleu de Prusse Rb0.94Mn[Fe (CN)6]0.98.0.3H2O, bistable à température ambiante. Par génération de second et de troisième harmonique, nous avons mesuré les non-linéarités effectives d’ordre deux et trois de ce composé dans les phases basse et haute température. Nous montrons que l’on peut faire photo-commuter les propriétés optiques linéaires et non linéaires de ce composé. La spectroscopie et la génération d’onde THz dans ce matériau sont également présentées et discutées<br>This thesis is dedicated to the study of laser-induced phase transitions in metallic and metaly organic materials. The studies presented here are guided by the recording and storage of digital information. Firstly, we focused on THz and Raman spectroscopy of two different iron Fe (II) spin crossover complexes. The spectra we recorded using these two methods are compared to numerical simulations obtained with the DFT. We have also studied the spin state transition induced byCO2 lasers in polymeric spin crossover materials. A simple experimental setup allowing data recording in this type of materials is presented. Secondly, we studied the reversible metal (λ metastable to semiconductor (β stable) phasetransition in nanoparticles of a Titanium oxide (Ti3O5), excited with nanosecond laser pulses.More specifically, we studied the kinetic aspects of this transition. It appears that the λ→β transition occurs in hundreds of nanoseconds while the β→λ transition is achieved in a few tens of nanoseconds. The photothermal mechanisms leading to this transition accounts very well to these experimental observations. Finally, we present the study of Rb0.94Mn[Fe (CN)6]0.98.0.3H2O, a Prussian blue analogue which is bistable at room temperature. Using secondy and thirdyharmonic generation, we measured the effective secondy and thirdyorder nonlinearities of this compound in low and high temperature phases. We show that we can photo-switch the linear and nonlinear optical properties of this material. THz spectroscopy and generation in this material are also presented
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Graber, Benjamin. "HIGH POWER TIME DOMAIN TERAHERTZ SPECTROSCOPY." Diss., Temple University Libraries, 2014. http://cdm16002.contentdm.oclc.org/cdm/ref/collection/p245801coll10/id/301211.
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Physics<br>Ph.D.<br>Terahertz (THz) has become a strong area for scientific research and commercial application in recent years. This research group has redesigned and optimized a THz photoconductive antenna, which currently operates with approximately 10x the power of a commercial antenna. It has been determined by this research that the THz signal emitted from a photoconductive antenna consists of coherent and incoherent signals. In addition to the improvement of the THz photoconductive antenna, I have optimized an electro optic THz detection system by characterizing the field dependency of an electro optic crystal, which enabled me to estimate the THz electric field strength. The high power THz source and optimized detection system were combined into a high power, high resolution time domain THz spectrometer. This spectrometer was used to conduct original measurements of the THz spectrum of water vapor, ionized air, and various chemical vapor including explosives. Most of these measurements were only possible with our improved THz spectrometer. In order to understand ionized air, an additional study was carried out to explore the ionization of several gases (e.g. N2, O2, Ar, CO2, and water vapor) which were ionized by radioactive isotopes. This unique study found that in addition to dose rate, the gamma energy of the radioactive isotopes and the sequential ionization levels of gases affect the equilibrium ion densities of these gases. This effect was especially pronounced for argon gas. The study of ion dynamics in gases has lead to the development of a prototype for stand-off detection and identification of radioactive isotopes. This prototype, despite being simple in design, can detect isotopes faster and more cheaply than a conventional gamma ray spectrometer. Throughout this thesis research I have successfully developed a high power, high resolution terahertz spectrometer and demonstrated that with the spectrometer I could identify characteristic resonances of water vapor, some chemicals including explosives, and even ionized air produced by nuclear isotopes. From the characteristic resonance frequencies one can understand the underlying physics or chemistry of molecules or atoms.<br>Temple University--Theses
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Yeh, Ka-Lo. "The generation of high field terahertz radiation and its application in terahertz nonlinear spectroscopy." Thesis, Massachusetts Institute of Technology, 2009. http://hdl.handle.net/1721.1/49748.
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Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2009.<br>Includes bibliographical references (p. 147-155).<br>In this thesis research, I implemented a terahertz generation scheme that enables high-field near-single-cycle terahertz (THz) pulse generation via optical rectification in a LiNbO3 (LN) crystal. I also developed a method for the non reconfigurable generation of high-intensity multiple-cycle THz fields aimed to more efficiently deliver THz energy to resonant samples. A novel free-space THz-pump/THz-probe setup enabled time-resolved measurement of ultrafast nonlinear electronic responses in doped bulk semiconductor samples. The ability to spectrally and temporally resolve the response of the semiconductor sample using a THz probe allowed us to uncover both the dynamics of impact ionization and interesting phonon-plasma interactions in indium antimonide (InSb) for the first time. Nonlinear vibrational responses in LN were ob-served first in a dual THz beam setup on an integrated LN waveguide platform with optical probing to reveal the generation of terahertz second harmonic signals and also in THz transmission measurements in cooled LN where THz intensity-dependent self-phase modulation and harmonic generation were observed. An outlook and preliminary results toward implementation and observation of high-field THz-driven responses in ferroelectric materials are given in the final chapter of this thesis.<br>by Ka-Lo Yeh.<br>Ph.D.
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Jones, Samuel Peter Philip. "Magneto-optics of complex oxides at terahertz frequencies." Thesis, University of Oxford, 2014. http://ora.ox.ac.uk/objects/uuid:c3d53c3c-d51a-417c-894a-fcb9681f1447.
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This thesis presents experimental results on two complex oxide systems: Cu<sub>1-x</sub>Zn<sub>x</sub>O and La<sub>0.7</sub>Sr<sub>0.3</sub>MnO<sub>3</sub>:ZnO. The dynamic magnetoelectric response of these materials is obtained using terahertz time-domain spectroscopy, supported by Fourier-transform infrared spectroscopy, Raman spectroscopy and X-ray diffraction. Evidence for an electromagnon in the multiferroic phase of CuO is presented for the first time. This high temperature (213-230K) electromagnon is linked to intersublattice exchange between two Cu sublattices. The temperature dependence of a magnon in the collinear antiferromagnetic phase is indicative of biquadratic exchange. Broadening of the multiferroic phase on substitution of copper with zinc is reported along with a 25% depression of the Néel temperature due to spin dilution. Phonons and magnons broaden and shift in energy on alloying. However, the electromagnon is relatively insensitive, increasing in energy without widening. This indicates that electromagnons and dynamic magnetoelectric coupling can be mantained even in disordered spin systems. Strong spin-phonon coupling is present in both magnetically ordered phases as shown by the anomalous behavior of the A<sup>3</sup><sub style='position: relative; left: -.5em;'>u</sub> phonon at T<sub>N1</sub> and a Raman-active mode associated with a magnetic modulation of a zone-folded acoustic phonon. Dynamic 1THz magnetoresistance is found to be significantly larger than static magnetoresistance in La<sub>0.7</sub>Sr<sub>0.3</sub>MnO<sub>3</sub>:ZnO vertically-aligned nanocolumns on LaAlO<sub>3</sub> substrates. The metal-insulator transition temperature is determined to be 300 K. Temperature dependent static and dynamic resistivity and magnetoresistance are discussed in terms of strain and grain boundary effects. Negative photoconductivity is observed and the dynamic response analysed.
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Knighton, Brittany E. "Nonlinear Ultrafast Excitation and Two-Dimensional Terahertz Spectroscopy of Solids." BYU ScholarsArchive, 2021. https://scholarsarchive.byu.edu/etd/9190.
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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.
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Wang, Yichao. "Terahertz nonlinear optical response of armchair graphene nanoribbons." Diss., University of Iowa, 2016. https://ir.uiowa.edu/etd/2163.
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It has become increasingly apparent that the future of next generation of electronic devices can and will rely on graphene nanoribbons. Graphene nanoribbons and sister structures showcase several key properties that can address the emerging need of terahertz science and technology, and break through the many technological limits on conventional semiconductor electronics operating in the terahertz spectrum.
In this thesis, we focus on the study of the terahertz nonlinear optical response of metallic armchair graphene nanoribbons and sister structures using a k.p model and time dependent perturbation theory. We find that these nanoribbons exhibit a stronger interband optical response, and a smaller critical field strength (of the order of 10 kV/m) than does 2D single layer graphene. We demonstrate that finite ribbon size, spatial profile of the applied terahertz radiation field, polarization of the applied terahertz radiation, a small band gap opening, and application of a superlattice potential are several ways to tune the strong terahertz nonlinear optical response of metallic armchair graphene nanoribbons.
The major contributions of this thesis include: 1) developes of a simpler method compared to other sophisticated methods of the terahertz nonlinear optical interband response of metallic armchair graphene nanoribbons; 2) extends the method in the characterization of various quantum size effects, elliptically polarized radiation field, small gap opening and superlattice on the terahertz optical response of these nanoribbons; 3) The versatility of the tunability showed in the terahertz nonlinear response of metallic armchair nanoribbons and sister structures will help advance the development of the nonlinear terahertz armchair graphene nanoribbon opto-electronic and photonic technology.
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Hwang, Harold Young. "Nonlinear terahertz spectroscopy of electronic and vibrational responses in condensed matter systems." Thesis, Massachusetts Institute of Technology, 2012. http://hdl.handle.net/1721.1/73174.
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Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2012.<br>This electronic version was submitted by the student author. The certified thesis is available in the Institute Archives and Special Collections.<br>Cataloged from student-submitted PDF version of thesis.<br>Includes bibliographical references.<br>In this work, I describe experiments utilizing high-field terahertz (THz) pulses to initiate nonlinear responses in several classes of materials. We have developed several methods for interrogating the nonlinear THz response of materials including collinear and noncollinear THz-pump/THz-probe spectroscopy, and THz-pump/optical probe spectroscopies including THz Kerr effect spectroscopy. We have observed nonlinear free-carrier absorption, occurring through the saturation of free-carrier mobility in bulk semiconductors. We have demonstrated that highly energetic electrons in the conduction band can generate electron-hole pairs in indium antimonide, and have elucidated the dynamics of the carrier generation process. We have observed nonlinear conductivity responses in graphene, showing that a strong THz pulse can heat the electron distribution leading to saturable absorption in the THz range. We have demonstrated THz-induced optical anisotropy in simple liquids, allowing for the measurement of subsequent orientational dynamics. We have driven nonlinear vibrational dynamics in ferroelectrics, demonstrating that the strong anharmonicity of lattice vibrational modes can induce an anisotropic optical response. We have begun to study nonlinear vibrational responses in molecular crystals, which is of importance in mode coupling and energy transfer processes in the THz range. Finally, we have driven nonlinear metamaterial responses in gallium arsenide and vanadium dioxide. In GaAs, we have shown that metamaterial properties may be tuned by an intense THz field if the substrate material (GaAs) is changed by the incident THz pulse, and we have demonstrated carrier multiplication locally in the metamaterial split ring resonator gaps where substantial electric field enhancement occurs. In VO2, we have shown that THz radiation can drive an insulator-to-metal phase transition, opening up new possibilities in the control of the states of matter with THz fields. This work has demonstrated only a few of the capabilities made possible by the interaction of intense THz radiation with matter, and provides a general framework to open up new research in a nascent field.<br>by Harold Young Hwang.<br>Ph.D.
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Xia, Chen. "Terahertz Time-Domain Spectroscopy of Low-Dimensional Materials and Photonic Structures." Case Western Reserve University School of Graduate Studies / OhioLINK, 2013. http://rave.ohiolink.edu/etdc/view?acc_num=case1355168322.
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Polyutov, Sergey. "Electron-nuclear Dynamics in Nonlinear Optics and X-ray spectroscopy." Doctoral thesis, Stockholm : Bioteknologi, Kungliga Tekniska högskolan, 2007. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-4339.
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Folland, Thomas. "Frequency control of terahertz quantum cascade lasers : theory and measurement." Thesis, University of Manchester, 2017. https://www.research.manchester.ac.uk/portal/en/theses/frequency-control-of-terahertz-quantum-cascade-lasers-theory-and-measurement(d4c55769-f053-4b79-aed3-e2fec575adde).html.
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Terahertz (THz) technology stands to solve a number of problems in everyday life, from next generation wireless communication to spectroscopic identification and imaging. However it is technically challenging to make a high power, compact source for terahertz radiation. The Quantum Cascade Laser (QCL), which produces gain at THz frequencies by exploiting inter-sub-band transitions in quantum wells, offers one solution to this problem. However controlling and detecting the emission from such sources remains a major challenge. This thesis investigates the theory and measurement of emission frequencies from aperiodic lattice THz QCLs. Crucially, realising both frequency control and detection provides a complete system for coherent THz characterisation of devices at precise, user defined frequencies. The author starts by studying the emission frequencies and threshold of discretely tuned aperiodic lattice lasers. This is achieved using a numerical transfer matrix method (TMM), which allows the calculation of the aperiodic lattice threshold spectrum for the first time. Calculations reveal that the low threshold modes of aperiodic lattice lasers form at peaks in the electromagnetic density of modes. This shows that lasing in aperiodic lattices arises from slow light propagation induced by multiple photonic band gaps, leading to both band edge and defect laser modes. Frequency selective lasing is maintained even under the influence of external facet feedback, albeit at the cost of precise knowledge of the mode frequency. Importantly this framework allows the understanding of essentially any aperiodic lattice laser system. Most significantly, the TMM is exploited in order to understand how graphene can be used to control a THz laser. Graphene interacts strongly with THz waves, and can be easily integrated with semiconductor structures such as lasers and waveguides. Here, numerical calculations reveal that graphene can be introduced into the waveguide of a THz QCL, generating electrically tunable THz surface plasmons. Such surface plasmons couple into an aperiodic lattice to change the scattering strength of each individual grating element. The TMM reveals that this change in scattering strength controls the modal selectivity of an aperiodic lattice THz QCL. This hypothesis successfully explains both earlier experiments and those performed by the author. Crucially, this model was central to a publication in the journal Science. Finally, this thesis demonstrates a novel coherent detection system for the characterisation of THz QCL emission. The technique exploits non-linear up-conversion of THz waves to a telecoms frequency side-band, a process shown to be sensitive to THz waveguide dispersion. By mixing the up-converted THz wave with a near infra-red local oscillator laser, coherent detection of QCL emission using all fibre coupled components is demonstrated for the first time. This measurement allows for the characterisation of laser emission with high frequency and temporal resolution. Specifically sub-microsecond pulses of THz emission and transients can be detected. When taken as a whole, the work of this thesis constitutes a major step towards realising cost effective THz characterisation and spectroscopy using QCLs.
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Jasper, Evan. "Development of Techniques in Time Domain Terahertz Spectroscopy for the Study of Chiral and Topological Materials." The Ohio State University, 2020. http://rave.ohiolink.edu/etdc/view?acc_num=osu1597048083501651.
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Liu, Ji-Cai. "Dynamics of multiphoton processes in nonlinear optics and x-ray spectroscopy." Doctoral thesis, KTH, Teoretisk kemi, 2009. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-11394.
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New generations of ultrashort and intense laser pulses as well ashigh power synchrotron radiation sources and x-ray free electronlasers have promoted fast developments in nonlinear optics andx-ray spectroscopy.The new experimental achievements and the appearance of varieties of novelnonlinear phenomena call for further development of theories. The objective of this thesis is to develop and apply thetheories to explain existing experimental data and to suggest new experiments. The first part of the thesis is devoted to nonlinear propagation of optical pulses. It is shown that the vibrational levels can be selectively populated by varying the duration, shape and intensity of the pump pulse. We obtained a strict analytical solution for the resonant two-photon interaction in a multilevel system beyond rotating wave approximation. Simulations show that the polarization anisotropy of the two-photon excitation affects strongly the anisotropy of photobleaching.The two-photon area theorem is reformulated with taking into account the dynamical Stark shift and the contribution from the permanent dipole moments. In general the dynamical Stark shift does not allow complete population of the excited state, but it can be compensated by detunings in atoms. A dynamical theory of the sequential two-photon absorption of microsecond pulses is developed to explore the role of transverse inhomogeneity of the light beam on optical limiting properties. The propagation of ultrashort laser pulses in nondipolar and dipolar media is investigated with special attention to the generation of superfluorescence and supercontinuum and the formation of attosecond pulses. The second part of the thesis addresses the interaction of molecules with x-ray radiation. We explore here the role of nuclear dynamics in resonant Auger scattering. Multimode simulations of the Auger spectra of ethylene molecule explain the main spectral features of the experimental spectra and show that the spectral profiles are formed mainly due to six vibrational modes. We predict the Doppler splitting of the atomic peak in resonant Auger scattering from SF6 molecule for circularly polarized x-rays. This effect is confirmed by the recent experiment. A new scheme of x-ray pump-probe spectroscopy, namely, resonant inelastic x-ray scattering accompanied by core-hole hopping induced by strong laser fields is suggested. The laser-induced promotion of core holes opens the symmetry forbidden scattering channels and gives rise to new spectral lines in the x-ray scattering spectrum. The strength of the symmetry forbidden lines becomes strong when the time of Rabi flopping is shorter than the lifetime of the core-excited state. We study the role of propagation of femtosecond x-ray free-electron pulses on the Auger process. Simulations show that there exists a strong competition between Auger decay and stimulated emission. The Auger yield and Auger branching ratio are strongly suppressed in the course of pulse propagation.<br>QC 20100729
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Kühn, Wilhelm [Verfasser], Elsässer [Akademischer Betreuer], Hamm [Akademischer Betreuer], and Masselink [Akademischer Betreuer]. "Nonlinear terahertz spectroscopy in one and two dimensions / Wilhelm Kühn. Gutachter: Elsässer ; Hamm ; Masselink." Berlin : Humboldt Universität zu Berlin, Mathematisch-Naturwissenschaftliche Fakultät I, 2011. http://d-nb.info/1015016944/34.
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Lim, Daeyoung. "Nonlinear optical spectroscopy of silicon-boron and other silicon-adsorbate systems." Access restricted to users with UT Austin EID Full text (PDF) from UMI/Dissertation Abstracts International, 2001. http://wwwlib.umi.com/cr/utexas/fullcit?p3034931.
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Metbulut, Mukaddes Meliz. "Development Of Compact Terahertz Time-domain Terahertz Spectrometer Using Electro-optic Detection Method." Master's thesis, METU, 2009. http://etd.lib.metu.edu.tr/upload/3/12610983/index.pdf.
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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.
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McGuckin, Brendan T. "Linear and nonlinear optical spectroscopy of semiconductors using opticallypumped lasers." Thesis, Heriot-Watt University, 1985. http://hdl.handle.net/10399/1655.
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Barlow, Aaron M. "Spectral Distortions & Enhancements In Coherent Anti-Stokes Raman Scattering Hyperspectroscopy." Thesis, Université d'Ottawa / University of Ottawa, 2015. http://hdl.handle.net/10393/32388.
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Coherent anti-Stokes Raman scattering microscopy is a versatile technique for label-free imaging and spectroscopy of systems of biophysical interest. Due to the coherent nature of the generated signals, CARS images and spectra can often be difficult to interpret. In this thesis, we document how distortions and enhancements can be produced in CARS hyperspectroscopy as a result of the instrument, geometrical optical effects, or unique molecular states, and discuss how these effects may be suppressed or exploited in various CARS applications.
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Valley, John Francis. "Nonlinear optical experiments in sodium vapor and comparison with Doppler-broadened two-level-atom theory." Diss., The University of Arizona, 1989. http://hdl.handle.net/10150/184930.
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Two spectral regions of gain exist for a weak probe beam propagating through a medium of two-level-atoms pumped by a strong near-resonance field. Experimentally a cw ring-dye laser is used to explore this gain at the Na D₂ resonance in a vapor. Plane-wave calculations of probe-gain spectra which include the Doppler broadening inherent in a vapor agree well with experimental spectra obtained with a Fabry-Perot interferometer. Such two-beam-coupling gain might have applications as optical pre- or power amplifiers. The gain is also the primary step in four-wave-mixing. Mixing of the pump and sideband which experiences gain produces the medium polarization from which the fourth-wave arises. For phase-matched propagation the fourth-wave, which is at a frequency that experiences little or negative probe-gain (i.e., absorption), grows at nearly the same rate as the primary sideband. Together the two sidebands extract far more than twice as much energy from the pump than does the primary sideband acting alone. Experimentally four-wave-mixing which arises from noise at the gain-sideband-frequency is sometimes accompanied by conical emission at the fourth-wave sideband. Since this sideband is also seen on axis the explanation cannot be simply phase-matching. Simulations which include the full transverse nature of the experiment are currently running on a CRAY supercomputer. These simulations indicate that the radial variation of the medium index of refraction is responsible for conical emission.
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Грідякіна, Олександра Валеріївна, and Аркадій Петрович Поліщук. "Nonlinear-optical recording in ionic liquid crystalline medium." Thesis, Physikzentrum in Bad Honnef, 2017. http://er.nau.edu.ua/handle/NAU/32390.
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Odhner, Johanan. "INVESTIGATIONS OF TEMPORAL RESHAPING DURING FILAMENTARY PROPAGATION WITH APPLICATION TO IMPULSIVE RAMAN SPECTROSCOPY." Diss., Temple University Libraries, 2012. http://cdm16002.contentdm.oclc.org/cdm/ref/collection/p245801coll10/id/196129.
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Chemistry<br>Ph.D.<br>Femtosecond laser filamentation in gaseous media is a new source of broadband, ultrashort radiation that has the potential for application to many fields of research. In this dissertation filamentation is studied with a view to understanding the underlying physics governing the formation and propagation dynamics of filamentation, as well as to developing a method for vibrational spectroscopy based on the filament-induced impulsive vibrational excitation of molecules in the filamentation region. In pursuit of a better understanding of the underlying physical processes driving filamentation, the development of a new method for characterizing high intensity ultrashort laser pulses is presented, wherein two laser beams generate a transient grating in a noble gas, causing the pulse undergoing filamentation to diffract from the grating. Measuring the spectrum as a function of time delay between the filament and probe beams generates a spectrogram that can be inverted to recover the spectral and temporal phase and amplitude of the filamentary pulse. This technique enables measurement of the filamentary pulse in its native environment, offering a window into the pulse dynamics as a function of propagation distance. The intrinsic pulse shortening observed during filamentation leads to the impulsive excitation of molecular vibrations, which can be used to understand the dynamics of filamentation as well. Combined measurements of the longitudinally-resolved filament Raman spectrum, power spectrum, and fluorescence intensity confirm the propagation dynamics inferred from pulse measurements and show that filamentation provides a viable route to impulsive vibrational spectroscopy at remote distances from the laser source. The technique is applied to thermometry in air and in flames, and an analytical expression is derived to describe the short-time dynamics of the rovibrational wave-packet dispersion experienced by diatomic molecules in the wave of the filament. It is found that no energy is initially partitioned into the distribution of rovibrational states during the filamentation process. Filament-assisted impulsive stimulated Raman spectroscopy of more complex systems is also performed, showing that filament-assisted vibrational measurements can be used as an analytical tool for gas phase measurements and has potential for use as a method for standoff detection. Finally, a study of the nonlinear optical mechanisms driving the filamentation process is conducted using spectrally-resolved pump-probe measurements of the transient birefringence of air. Comparison to two proposed theories shows that a newly described effect, ionization grating-induced birefringence, is largely responsible for saturation and sign inversion of the birefringence at 400 nm and 800 nm, while the magnitude of contributions described by a competing theory that relies on negative terms in the power series expansion of the bound electron response remain undetermined.<br>Temple University--Theses
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Hu, Zhen Kimble H. Jeff Kimble H. Jeff. "Quantum optics with cold atoms--nonlinear spectroscopy and road toward single-atom trap /." Diss., Pasadena, Calif. : California Institute of Technology, 1995. http://resolver.caltech.edu/CaltechETD:etd-10112007-092812.
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Folpini, Giulia. "Exploring Nonresonant Interactions in Condensed Matter by Two-Dimensional Terahertz Spectroscopy." Doctoral thesis, Humboldt-Universität zu Berlin, 2018. http://dx.doi.org/10.18452/18860.
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Zur Untersuchung nichtlinearer Reaktionen von kondensierten Materie-Systemen wird die multidimensionale Terahertz-Spektroskopie genutzt.
Ein mehrere Oktaven umfassende THz-Quelle, die auf der Frequenzmischung in organischen Kristallen basiert, wird entwickelt und zur Erforschung der Librationsbande von Wasser-Nanotröpfchen in DOPC-Micellen verwendet.
Die nichtresonante THz-Strahlung wird genutzt, um die Emission im mittleren Infrarotbereich eines Intersubband-Übergangs von GaAs-Quantentöpfen kohärent zu steuern.
Schließlich wird die 2D-THz-Spektroskopie verwendet, um die nichtlineare Antwort einer "soft-mode" in einem Aspirin-Molekül-Kristall zu studieren.<br>Multidimensional Terahertz spectroscopy is used to investigate the nonlinear response of condensed matter systems. A multioctave-spanning THz source based on frequency mixing in organic crystals is developed and used to study the libration band of water nanodroplets confined in DOPC micelles. Nonresonant THz radiation is used to coherently control the mid-infrared emission of an intersubband transition of GaAs quantum wells. Finally, 2D THz spectroscopy is used to study the nonlinear response of a soft mode in an aspirin molecular crystal.
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Govani, Jayesh R. "Spectroscopic characterizations of organic/inorganic nanocomposites." To access this resource online via ProQuest Dissertations and Theses @ UTEP, 2009. http://0-proquest.umi.com.lib.utep.edu/login?COPT=REJTPTU0YmImSU5UPTAmVkVSPTI=&clientId=2515.
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Sinha, Raju. "Tunable, Room Temperature THz Emitters Based on Nonlinear Photonics." FIU Digital Commons, 2017. http://digitalcommons.fiu.edu/etd/3172.
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The Terahertz (1012 Hz) region of the electromagnetic spectrum covers the frequency range from roughly 300 GHz to 10 THz, which is in between the microwave and infrared regimes. The increasing interest in the development of ultra-compact, tunable room temperature Terahertz (THz) emitters with wide-range tunability has stimulated in-depth studies of different mechanisms of THz generation in the past decade due to its various potential applications such as biomedical diagnosis, security screening, chemical identification, life sciences and very high speed wireless communication. Despite the tremendous research and development efforts, all the available state-of-the-art THz emitters suffer from either being large, complex and costly, or operating at low temperatures, lacking tunability, having a very short spectral range and a low output power. Hence, the major objective of this research was to develop simple, inexpensive, compact, room temperature THz sources with wide-range tunability.
We investigated THz radiation in a hybrid optical and THz micro-ring resonators system. For the first time, we were able to satisfy the DFG phase matching condition for the above-mentioned THz range in one single device geometry by employing a modal phase matching technique and using two separately designed resonators capable of oscillating at input optical waves and generated THz waves. In chapter 6, we proposed a novel plasmonic antenna geometry – the dimer rod-tapered antenna (DRTA), where we created a hot-spot in the nanogap between the dimer arms with a very large intensity enhancement of 4.1×105 at optical resonant wavelength. Then, we investigated DFG operation in the antenna geometry by incorporating a nonlinear nanodot in the hot-spot of the antenna and achieved continuously tunable enhanced THz radiation across 0.5-10 THz range. In chapter 8, we designed a multi-metallic resonators providing an ultrasharp toroidal response at THz frequency, then fabricated and experimentally demonstrated an efficient polarization dependent plasmonic toroid switch operating at THz frequency.
In summary, we have successfully designed, analytically and numerically investigated novel THz emitters with the advantages of wide range tunability, compactness, room temperature operation, fast modulation and the possibility for monolithic integration, which are the most sought after properties in the new generation THz sources.
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Robertson, John Michael. "Nonlinear optical properties of absorbing molecular systems." Thesis, University of Essex, 2002. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.390961.
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Бордюг, Ганна Борисівна, and Аркадій Петрович Поліщук. "Fast photoconversion in viologen-doped lyotropic ionic liquid crystals." Thesis, Physikzentrum in Bad Honnef, 2017. http://er.nau.edu.ua/handle/NAU/32391.
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Liang, Qijun [Verfasser]. "Terahertz Time-Domain Spectroscopy : Characterization of Nonlinear Crystals, Nanowires, 2D Gratings,Organic Liquids, and Polystyrene Particles / Qijun Liang." Konstanz : Bibliothek der Universität Konstanz, 2015. http://d-nb.info/1110772335/34.
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Leigh, Matthew. "HIGH POWER PULSED FIBER LASER SOURCES AND THEIR USE IN TERAHERTZ GENERATION ." Diss., The University of Arizona, 2008. http://hdl.handle.net/10150/193797.
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In this dissertation I report the development of high power pulsed fiber laser systems. These systems utilize phosphate glass fiber for active elements, instead of the industry-standard silica fiber. Because the phosphate glass allows for much higher doping of rare-earth ions than silica fibers, much shorter phosphate fibers can be used to achieve the same gain as longer silica fibers.This single-frequency laser technology was used to develop an all-fiber actively Q-switched fiber lasers. A short cavity is used to create large spacing between longitudinal modes. Using this method, we demonstrated the first all-fiber Q-switched fiber laser in the 1 micron region.In addition to creating high peak powers with Q-switched lasers, created even higher powers using fiber amplifier systems. High power fiber lasers typically produce spectral broadening through the nonlinear effects of stimulated Raman scattering, stimulated Brullion scattering, and self-phase modulation. The thresholds for these nonlinearities scale inversely with intensity and length. Thus, we used a short phosphate fiber gain stage to reduce the length, and a large core fiber final stage to reduce intensity. In this way we were able to generate high peak power pulses while avoiding visible nonlinearities, and keeping a narrow bandwidth.The immediate goal of developing these high power fiber laser systems was to generate narrowband terahertz radiation. Two different wavelengths were combined into the final amplifier stage at orthogonal polarizations. These were collimated and directed into a GaSe crystal, which has a very high figure of merit for THz generation. The two wavelengths combined in the crystal through the process of nonlinear difference frequency generation. This produced a narrowband beam of THz pulses, at higher powers than previous narrowband THz pulses produced by eyesafe fiber lasers.
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Turksen, Zeynep. "Applications In Broadband Thz Spectroscopy Towards Material Studies." Master's thesis, METU, 2011. http://etd.lib.metu.edu.tr/upload/12612908/index.pdf.
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The purpose of this work was to construct and analyze a THz time domain spectroscopy (THz-TDS) system by using a nanojoule energy per pulse ultrafast laser (non-amplified ultrafast laser or oscillator) source and a non-linear optical generation method for THz generation. First a THz-TDS system, which uses photoconductive antenna (PCA) method for THz generation, was built to understand the working principles of these types of systems. This THz-TDS system which used PCA for generation and a 2mm thick <<br>110><br>ZnTe crystal for detection had a bandwidth up to 1 THz with a 1000:1 signal to noise ratio (S/N). Using this system, various materials were investigated to study the usefulness of the obtained bandwidth. Absorption coefficient and refractive indices of the sample materials were calculated. Results showed that the bandwidth of the system was not sufficient to obtain fingerprint properties of these materials. In order to improve the system, optical rectification method was used for THz generation. A different THz-TDS system was built with a 1mm thick <<br>110><br>ZnTe crystal used for the method of non-linear generation of THz radiation. Theoretical calculations of radiated intensity and electric field were done to analyze the expected bandwidth of the system. Results showed that the generation and the detection crystal thicknesses affect the obtained bandwidth of the system in that the bandwidth limiting factor is the crystal thickness and not the ultrafast laser pulse duration. Especially for detection, measurements obtained with both a 1mm thick and 2mm thick <<br>110><br>ZnTe crystal showed that there was not much difference in bandwidth as was predicted by theory. Also in order to increase the signal to noise ratio, the optics used in the system were optimized. It was found that by using same focal lengths for focusing and collimating optics around the generation crystal and by using a short focal length parabolic mirror, S/N could be improved. After these improvements this THz-TDS system which uses optical rectification for THz generation and electro-optic method for THz detection had a larger bandwidth up to 3 THz but with a lower 100:1 signal to noise ratio.
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Грідякіна, Олександра Валеріївна, and Ганна Борисівна Бордюг. "Nonlinear helical winding in highly viscous chiral thin films." Thesis, NANO-2017, 2017. http://er.nau.edu.ua/handle/NAU/32389.
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Herman, Gregory S. "Terahertz Local Oscillator Via Difference Frequency Generation in III-V Semiconductors Using Frequency Stabilized Lasers." Diss., The University of Arizona, 2013. http://hdl.handle.net/10150/306995.
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Terahertz (THz) heterodyne receiver systems are required by NASA to monitor gas concentrations related to the Earth's ozone depletion. To this end, NASA needs compact, solid state, tunable THz local oscillators. THz LOs have been developed using three means: 1) All-electronic LOs using mixers in combination with Gunn oscillators, 2) Hybrid Photo-electronic LOs using a cw analog of the Auston switch, and 3) All-photonic THz LOs using coherent sources, such as vapor lasers or solid-state Quantum Cascade Lasers, and down converting lasers using nonlinear crystals. In this dissertation, we began with two frequency stabilized Nd:YAG lasers, locked to a common reference cavity, as a starting point to having a stable input into a nonlinear optical frequency conversion system. Following this, we explored the nonlinear crystals useful for THz generation, and the phasematching schemes that could be employed by each. We concluded by settling on highly insulating III-V semiconductor crystals as the proper choice of nonlinear element, and put together a new phasematching method that is most useful for them.
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Kimberg, Victor. "Pulse Propagation in Nonlinear Media and Photonic Crystals." Doctoral thesis, Stockholm, 2006. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-3886.
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Fu, Jie. "Molecular Structure-Nonlinear Optical Property Relationships for a Series of Polymethine and Squaraine Molecules." Doctoral diss., University of Central Florida, 2006. http://digital.library.ucf.edu/cdm/ref/collection/ETD/id/3941.
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This dissertation reports on the investigation of the relationships between molecular structure and two-photon absorption (2PA) properties for a series of polymethine and squaraine molecules. Current and emerging applications exploiting the quadratic dependence upon laser intensity, such as two-photon fluorescence imaging, three-dimensional microfabrication, optical data storage and optical limiting, have motivated researchers to find novel materials exhibiting strong 2PA. Organic materials are promising candidates because their linear and nonlinear optical properties can be optimized for applications by changing their structures through molecular engineering. Polymethine and squaraine dyes are particularly interesting because they are fluorescent and showing large 2PA. We used three independent nonlinear spectroscopic techniques (Z-scan, two-photon fluorescence and white-light continuum pump-probe spectroscopy) to obtain the 2PA spectra revealing 2PA bands, and we confirm the experimental data by comparing the results from the different methods mentioned. By systematically altering the structure of polyemthines and squaraines, we studied the effects of molecular symmetry, strength of donor terminal groups, conjugation length of the chromophore chain, polarity of solvents, and the effects of placing bridge molecules inside the chromophore chain on the 2PA properties. We also compared polymethine, squaraine, croconium and tetraon dyes with the same terminal groups to study the effects of the different additions inserted within the chromophore chain on their optical properties. Near IR absorbing squaraine dyes were experimentally observed to show extremely large 2PA cross sections ([approximately equal to] 30000GM). A simplified three-level model was used to fit the measured 2PA spectra and detailed quantum chemical calculations revealed the reasons for the squaraine to exhibit strong 2PA. In addition, two-photon excitation fluorescence anisotropy spectra were measured through multiple 2PA transitions. A theoretical model based on four-levels with two intermediate states was derived and used for analysis of the experimental data.<br>Ph.D.<br>Other<br>Optics and Photonics<br>Optics
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Averett, Shawn C. "Advancements in the Understanding of Nonlinear Optics and Their Use in Material Analysis." BYU ScholarsArchive, 2017. https://scholarsarchive.byu.edu/etd/6507.
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Adhesion, heterogeneous catalysis, electrochemistry, and many other important processes and properties are driven by interactions at surfaces and interfaces. Vibrational sum frequency generation spectroscopy (VSFG) is an increasingly popular analytical technique because it can provide information about the nature and physical orientation of functional groups at these surfaces and interfaces. Analysis of VSFG data can be complicated by the presence of SFG signal that is not associated with a resonant vibration. This nonresonant sum frequency generation (NR-SFG) signal can interfere with the resonant signal and influence the detected spectrum. Methods have been developed to remove NR-SFG signal; however, these methods tend to be complicated and expensive. In fact many SFG practitioners do not have the ability to remove NR-SFG signal components, and systems designed to remove NR-SFG signal contributions may not be able to do so for some materials. We have worked to help develop a better understanding of NR-SFG. As part of this work, a better understanding of the temporal and phase behavior of NR-SFG signal has been developed, based on the behavior of NR-SFG signal from Si(111) wafers. This work calls into question some assumptions underlying nonresonant suppression methods based on time-domain detection. A new method for nondestructively testing (NDT) materials has been developed that uses nonresonant second harmonic generation, the degenerate form of SFG. This new NDT technology has the potential to detect several forms of material damage, such as aluminum sensitization, and plastic deformation of materials, which are largely invisible to current NDT technologies. Methods for extracting functional group orientation from VSFG data that contains NR-SFG contributions are also demonstrated and used to investigate how the surface of high density polyethylene changes in response to mechanical deformation. This work shows that the inability to remove NR-SFG contributions from VSFG spectra does not mean that these instruments cannot be used to make important discoveries. It simply means that NR-SFG contributions must be properly understood and accounted for during experimental design, and kept in mind during the analysis of VSFG spectra.
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Olszak, Peter D. "Nonlinear absorption and free carrier recombination in direct gap semiconductors." Doctoral diss., University of Central Florida, 2010. http://digital.library.ucf.edu/cdm/ref/collection/ETD/id/4620.
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Nonlinear absorption of Indium Antimonide (InSb) has been studied for many years, yet due to the complexity of absorption mechanisms and experimental difficulties in the infrared, this is still a subject of research. Although measurements have been made in the past, a consistent model that worked for both picosecond and nanosecond pulse widths had not been demonstrated. In this project, temperature dependent two-photon (2PA) and free carrier absorption (FCA) spectra of InSb are measured using femtosecond, picosecond, and nanosecond IR sources. The 2PA spectrum is measured at room temperature with femtosecond pulses, and the temperature dependence of 2PA and FCA is measured at 10.6[micro]meters using a nanosecond CO[sub]2 laser giving results consistent with the temperature dependent measurements at several wavelengths made with a tunable picosecond system. Measurements over this substantial range of pulse widths give results for FCA and 2PA consistent with a recent theoretical model for FCA. While the FCA cross section has been generally accepted in the past to be a constant for the temperatures and wavelengths used in this study, this model predicts that it varies significantly with temperature as well as wavelength. Additionally, the results for 2PA are consistent with the band gap scaling (Eg[super]-3) predicted by a simple two parabolic band model. Using nanosecond pulses from a CO?éé laser enables the recombination rates to be determined through nonlinear transmittance measurements. Three-photon absorption is also observed in InSb for photon energies below the 2PA band edge. Prior to this work, data on three-photon absorption (3PA) in semiconductors was scarce and most experiments were performed over narrow spectral ranges, making comparison to the available theoretical models difficult. There was also disagreement between the theoretical results generated by different models, primarily in the spectral behavior.; Therefore, we studied the band gap scaling and spectra of 3PA in several semiconductors by the Z-scan technique. The 3PA coefficient is found to vary as (Eg[super]-7), as predicted by the scaling rules of simple two parabolic band models. The spectral behavior, which is considerably more complex than for 2PA, is found to agree well with a recently published theory based on a four-band model.<br>ID: 029050684; System requirements: World Wide Web browser and PDF reader.; Mode of access: World Wide Web.; Thesis (Ph.D.)--University of Central Florida, 2010.; Includes bibliographical references.<br>Ph.D.<br>Doctorate<br>Optics and Photonics
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Ford, William Paul. "Development of a Fourier Transform Far Infrared (FTFIR) Spectrometer to Characterize Broadband Transmission Properties of Common Materials in the Terahertz Region." Wright State University / OhioLINK, 2006. http://rave.ohiolink.edu/etdc/view?acc_num=wright1158508606.
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Shah, Anjali. "External cavity diode lasers and non-linear optical frequency conversion in spectroscopic applications." Thesis, St Andrews, 2006. http://hdl.handle.net/10023/142.
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Peceli, Davorin. "Absorptive and Refractive Optical Nonlinearities in Organic Molecules and Semiconductors." Doctoral diss., University of Central Florida, 2013. http://digital.library.ucf.edu/cdm/ref/collection/ETD/id/5687.
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The main purpose of this dissertation to investigate photophysical properties, third order nonlinearity and free carrier absorption and refraction in organic materials and semiconductors. Special emphasis of this dissertation is on characterization techniques of molecules with enhanced intersystem crossing rate and study of different approaches of increasing triplet quantum yield in organic molecules. Both linear and nonlinear characterization methods are described. Linear spectroscopic characterization includes absorption, fluorescence, quantum yield, anisotropy, and singlet-oxygen generation measurements. Nonlinear characterization, performed by picosecond and femtosecond laser systems (single and double pump-probe and Z-scan measurements), includes measurements of the triplet quantum yields, excited-state absorption, two-photon absorption, nonlinear refraction and singlet and triplet-state lifetimes. The double pump-probe technique is a variant of the standard pump-probe method but uses two pumps instead of one to create two sets of initial conditions for solving the rate equations allowing a unique determination of singlet- and triplet-state absorption parameters and transition rates. The advantages and limitations of the the double pump-probe technique are investigated theoretically and experimentally, and the influences of several experimental parameters on its accuracy are determined. The accuracy with which the double pump-probe technique determines the triplet-state parameters improves when the fraction of the population in the triplet state relative to the ground state is increased. Although increased accuracy is in principle achievable by increasing the pump fluence in the reverse saturable absorption range, it is shown that the DPP is optimized by working in the saturable absorption regime. Two different approaches to increase intersystem crossing rates in polymethine-like molecules are presented: traditional heavy atom substitution and molecular levels engineering. Linear and nonlinear optical properties of a series of polymethine dyes with Br- and Se- atoms substitution, and a series of new squaraine molecules, where one or two oxygen atoms in a squaraine bridge are replaced with sulfur atoms, are investigated. A consequence of the oxygen-to-sulfur substitution in squaraines is the inversion of their lowest lying ??' and n?' states leading to a significant reduction of singlet-triplet energy difference and opening of an additional intersystem channel of relaxation. Experimental studies show that triplet quantum yields for polymethine dyes with heavy-atom substitutions are small (not more than 10%), while for sulfur-containing squaraines these values reach almost unity. Experimental results are in agreement with density functional theory calculations allowing determination of the energy positions, spin-orbital coupling, and electronic configurations of the lowest electronic transitions. For three different semiconductors: GaAs, InP and InAsP two photon absorption, nonlinear refraction and free carrier absorption and refraction spectrums are measured using Z-scan technique. Although two photon absorption spectrum agrees with the shape of theoretical prediction, values measured with picosecond system are off by the factor of two. Nonlinear refraction and free carrier nonlinearities are in relatively good agreement with theory. Theoretical values of the third order nonlinearities in GaAs are additionally confirmed with femtosecond Z-scan measurements. Due to large spectral bandwidth of femtosecond laser, three photon absorption spectrum of GaAs was additionally measured using picosecond Z-scan. Again, spectral shape is in excellent agreement with theory however values of three photon absorption cross sections are larger than theory predicts. ?<br>Ph.D.<br>Doctorate<br>Optics and Photonics<br>Optics and Photonics<br>Optics
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Delmonte, Valentin. "Spectroscopie cohérente des excitons dans des nanostructures semi-conductrices innovantes." Thesis, Université Grenoble Alpes (ComUE), 2018. http://www.theses.fr/2018GREAY015/document.
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L'évolution des technologies liées aux semi-conducteurs a amené à l'étude de la cohérence des Bits Quantiques (Qbits) dans l'objectif de réduction de la taille des composants. A l'aide de la spectroscopie cohérente non-linéaire, j'ai pu étudier les propriétés de cohérences des excitons confinés dans des boites quantiques (BQ), eux-même intégrées dans différentes nano-structures. L'intérêt des nano-structures est d'augmenter le ratio signal-sur-bruit, indispensable dans notre expérience. L'utilisation des nano-structures est aussi indispensable dans l'objectif de la mise en place d'un couplage radiatif à longue distance entre 2 BQs. Il fut tout d'abord nécessaire de caractériser des nano-structures déterministes permettant d'augmenter le rendement d 'échantillons utilisables en conservant l'intensité de signal émit par les BQs. De plus, j'ai développé mon expérience afin d'affiner notre capacité d'étudier le couplage proches entre BQs intégrées dans une micro-cavité. Ensuite Nous avons testé plusieurs formes de nano-structures 1D (trompettes et ridges) afin de d'amplifier le couplage à longue distance et et comprendre les obstacles auxquels nous auront à faire face . Enfin une caractérisation de nouveaux matériaux 2D fut réalisée, en vue de d'améliorer notre compréhension des dynamiques des excitons dans ce type de matériaux<br>The evolution of technologies related to semiconductors has led to the study of the coherence of Quantum Bits (Qbits) in order to reduce the size of the components. Using nonlinear coherent spectroscopy, I was able to study the coherence properties of excitons confined in quantum dots (BQs), themselves integrated into different nano-structures. The interest of nanostructures is to increase the signal-to-noise ratio, essential in our experience. The use of nano-structures is also essential for the purpose of setting up a long-distance radiative coupling between 2 BQs.First of all, it was necessary to characterize deterministic nano-structures that make it possible to increase the yield of usable samples by preserving the signal intensity emitted by the BQs. In addition, I developed my experience to refine our ability to study close-coupling between BQs embedded in a micro-cavity. Then we tested several forms of 1D nano-structures (trumpets and ridges) in order to amplify the long-distance coupling and to understand the obstacles we will have to face. Finally a characterization of new 2D materials was realized, in order to improve our understanding of exciton dynamics in this type of materials
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Thomson, Caroline L. "Study of phase-matching geometries in bulk and periodically-poled lithium niobate and their use in intracavity terahertz optical parametric oscillators." Thesis, University of St Andrews, 2012. http://hdl.handle.net/10023/3024.
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This thesis describes the experimental implementation of novel intersecting cavity terahertz optical parametric oscillators based on bulk and periodically-poled magnesium oxide-doped lithium niobate. Both collinear and non-collinear phase-matching geometries have been demonstrated and injection-seeding has been implemented in devices using periodically-poled material to reduce threshold and increase the down-conversion efficiency. A comprehensive characterisation of the original intracavity terahertz OPO was undertaken, which revealed the parameters having the greatest impact on OPO efficiency (idler mirror reflectivity and cavity length) and led to a better understanding of the losses in the system. During the characterisation process, generation of further terahertz radiation at the same frequency as that generated by the parametric process was observed and identified as being a result of difference frequency generation (DFG) between the parametrically-generated idler and terahertz waves. This phenomenon had previously only been observed when periodically-poled materials were employed in the system. The effect of this additional DFG process has been analysed in terms of the enhancement of the terahertz field on the basis of the coupled wave equations and physically measured quantities. The use of periodically-poled lithium niobate has been a major part of the research presented in this thesis. A comprehensive study of the modified phase-matching conditions was carried out and both collinear and novel hybrid non-collinear phase-matching geometries were identified. Several computer models were developed to assess the performance of any given grating design in these different geometries and the effects of temperature tuning and pump wavelength variation were also investigated using the models. Experimental studies confirmed the viability of the modelling approach but material limitations (particularly the early onset of crystal damage) limited the outcomes of the experiments. A detailed comparison of the poled and bulk materials was made to highlight the present drawbacks of the poled material. Finally, injection seeding was used to improve the efficiency of the collinear phase-matched PPLN OPOs. When seeding was used the depletion of the pump pulse was increased to the point of being measurable, reaching an upper level of 10%. Coupling constraints placed on the seed laser limited the amount of depletion attained. The potential for injection seeding to be used in the hybrid non-collinear phase-matching scheme was also identified but not realised during the course of this work. Were this technique successful, the tuning range of the intersecting cavity terahertz OPO could be extended to encompass the sub-1THz region, something that has previously been limited by the available idler cavity angles.
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Johnson, Magnus. "Vibrational Sum Frequency and Infrared Reflection/Absorption Spectroscopy Studies of the Air/Liquid and Liquid/Metal Interfaces." Doctoral thesis, Stockholm, 2005. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-455.
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Isaienko, Oleksandr. "Development of ultra-broadband ultrafast infrared sources and applications to nonlinear vibrational spectroscopy of interfaces." Diss., Temple University Libraries, 2011. http://cdm16002.contentdm.oclc.org/cdm/ref/collection/p245801coll10/id/141408.
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Chemistry<br>Ph.D.<br>Interfaces play a crucial role in the exchange of energy and matter in various physical, chemical and biological systems. A particular interest has been to study interfaces between aqueous phases and various minerals because of their importance in understanding geochemical phenomena as well as for applications such as enhanced oil recovery. The nonlinear optical technique of vibrational sum-frequency generation (SFG) spectroscopy, introduced over 20 years ago, has become a powerful tool to investigate various surfaces, in particular, mineral-water interfaces. One of the challenges of the SFG spectroscopy of aqueous surfaces is the need to tune the central frequency of relatively narrowband IR lasers through the broad range of the OH-stretch frequencies of water molecules (3000 - 4000 cm-1). We have developed a novel ultrabroadband IR laser source that generates infrared pulses in the ~2800-6000 cm-1 range (lambda~3300-1800 nm) with bandwidths Delta(nu)>1000 cm-1, and bandwidths >2000 cm-1 in the near-IR range (lambda~1000-2000 nm). Pulse front tilt of signal pulse has been corrected allowing for compression of signal pulses down to 25 fsec. Such ultrabroadband IR pulses allow us to perform SFG spectroscopy of aqueous surfaces over the entire frequency range of water molecule spectrum (extending from ~2900 cm -1 to ~3800 cm -1) simultaneously, without tuning the laser ("in one shot"). We have used this novel ultrabroadband IR source to investigate the vibrational SFG spectra of silica/water interfaces. The high signal-to-noise ratio of our spectroscopic setup has allowed us to study low-intensity features that were not studied in detail, or recognized previously in the SFG-spectroscopy investigations, including: 1) non-hydrogen bonded OH vibrations at hydrophilic silica/water interfaces; 2) combination [stretch+bend] bands of water at the silica surface appearing at ~5000-5200 cm -1. 3) Overtones of water stretching modes at silica/water interfaces. The most important conclusions from these studies are outlined below. 1. Non-hydrogen bonded hydroxyls at silica/water interface. Typically SFG-studies of mineral/water interfaces (in particular, silica/water) have focused on the most pronounced features - peaks of H-bonded hydroxyls at ~3150 and ~3450 cm -1. We have been able to systematically observe and study a weaker peak at ~3670 - 3700 cm -1. This peak becomes more pronounced as the pH of aqueous phase decreases, as well as the ionic strength increases, indicating that the hydroxyls corresponding to this spectral feature are situated in a very close proximity to the surface. Isotopic dilution experiments indicate that the 3700 cm -1 feature is not due to asymmetric OH stretches as was suggested before. Based on our results, we suggest that this spectral feature corresponds to hydroxyls of water molecules at the silica surface that cannot hydrogen bond with silanol groups because of the lower density of silanols compared to H2O. We believe this to be the first surface-specific study of non-hydrogen bonded hydroxyls at silica, a surface widely accepted as hydrophilic. 2. SFG spectroscopy of [ν(OH)+δ(HOH)] combination bands of water at silica surface. We have extended SFG spectroscopy of the interfacial hydroxyls at mineral/water surfaces into the near-IR frequency range. The studies of overtones of interfacial OH(OD) groups will provide information on the anharmonicity of such species, and thus on the energy of dissociation. In addition, the positions of the overtone frequencies of the hydroxyls are more sensitive to interactions with the environment than the fundamental stretch frequencies. Our particular focus has been to study the stretch+bend combination band nu comb nu;(OH)+delta;(HOH) of liquid water which occurs in the near-IR spectral range at ~5000-5200 cm -1. It is typically much weaker in the FTIR absorption spectra than the fundamental transitions of the OH stretches or HOH bending, similar to overtones of these modes. We have performed, what we believe to be, the first surface-specific vibrational SFG spectroscopic measurements of combination bands of water molecules at silica surfaces. SFG spectroscopy of water combination band allows access to the water bending mode (delta~1600 cm -1), which still has not been observed in sum-frequency.<br>Temple University--Theses
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Поліщук, Аркадій Петрович, Олександра Валеріївна Грідякіна, and Ганна Борисівна Бордюг. "Matrix effec on the electrooptical properties of heptylviologen." Thesis, XXIII ISSSMC, 2017. http://er.nau.edu.ua/handle/NAU/32388.
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