Le travail de thèse présenté dans ce manuscrit traite des lasers à cascade quantique à plasmons de surface dans la gamme spectrale du moyen-IR et de leurs applications aux cristaux photoniques moyen-IR et THz. Pour les grandes longueurs d'onde (λ > 10µm) la lumière est confinée au sein de la région active du laser grâce à une couche de métal déposée directement à la surface de la région active. Ces guides sont appelés guide à plasmons de surface. La faible épaisseur de ces guides est un atout majeur pour la fabrication de dispositifs à cristal photonique ou DFB (Distributed Feed Back). Ce manuscrit présente une étude complète de ces guides. Il démontre de manière expérimentale et théorique qu'il est possible d'améliorer les performances de ces guides en utilisant une couche d'argent à la place de l'or habituellement utilisé. Pour approfondir cette étude, une méthode originale basée sur les guides multisections et permettant de mesurer les pertes et le gain des guides à plasmons de surface a été soigneusement étudiée à l'aide de nombreuses expériences. La deuxième partie de ce manuscrit est consacrée à l'étude théorique du réseau nid d'abeille pour la fabrication de microcavité laser pour le moyen-IR et le THz. Cette étude est réalisée grâce à des simulations bidimensionnelles à partir d'un code utilisant la méthode des ondes planes et en trois dimensions grâce à un code utilisant la méthode FDTD (Finite-Difference Time-Domain). Lors de ces études, un phénomène nouveau a été mis en évidence sur les guides métal-métal THz démontrant qu'il est possible d'implémenter un cristal photonique par la seule structuration du métal du contact supérieur.

Dye-sensitized solar cells (DSSCs) and perovskite solar cells are emerging as promising potential low-cost alternatives to established crystalline silicon photovoltaics. Of the employed functional materials, however, many fundamental optoelectronic properties governing photovoltaic device operation are not sufficiently well understood. This thesis reports on a series of studies using ultrafast THz and photoluminescence spectroscopy on two classes of such materials, providing insight into the dynamics of charge-transport and recombination processes following photoexcitation. For TiO₂-nanotubes, which have been proposed as easy-to-fabricate electron transporters for DSSCs, fast, shallow electron trapping is identified as a limiting factor for efficient charge collection. Trapping lifetimes are found to be about an order of magnitude shorter than in the prevalently employed sintered nanoparticles under similar excitation conditions and trap saturation effects are not observed, even at very high excitation densities. In organo-lead halide perovskites - specifically CH₃NH₃PbI₃ and CH₃NH₃PbI_3-xCl_x, which have only recently emerged as highly efficient absorbers and charge transporters for thin-film solar cells, carrier mobilities and fundamental recombination dynamics are revealed. Extremely low bi-molecular recombination rates at least four orders of magnitude below the prediction of Langevin's model are found as well as relatively high charge-carrier mobilities in comparison to other solution-processable materials. Furthermore a very low influence of trap-mediated recombination channels was observed. Due to a combination of these factors, diffusion lengths reach hundreds of nanometres for CH₃NH₃PbI₃ and several microns for CH₃NH₃PbI_3-xCl_x. These results are shown to hold for both, solution processed and vapour-deposited CH₃NH₃PbI_3-xCl_x and underline the superb suitability of the materials as absorbers in solar cells, even in planar heterojunction architectures. The THz-frequency spectrum of the conductivity of the investigated perovskites is consistent with Drude-like charge transport additionally exhibiting weak signatures of phonon coupling. These coupling effects are also reflected in the luminescence of CH₃NH₃PbI_3-xCl_x, where they are believed to be the cause of the observed homogeneous spectral broadening. Further photoluminescence measurements were performed at temperatures between 4 K and room temperature to study the nature of recombination pathways in the material.

La gamme térahertz est une région du spectre électromagnétique située à l'interface entre les techniques optiques et électroniques de génération et de détection d'un rayonnement. Elle est qualifiée de "fossé" technologique THz en raison du manque de dispositifs alors que les applications potentielles concernant cette gamme sont vastes. Cette thèse comporte trois axes de recherches articulés autour d'une source THz prometteuse : les lasers à cascade quantique (LCQ). Ces hétérostructures de semiconducteurs sont des lasers unipolaires dont l'émission repose sur la relaxation d'électrons entre des états con nés de la bande de conduction (transitions intersousbandes). Tout d'abord, un système de spectroscopie THz dans le domaine temporel, adapté à l'étude du spectre du gain des LCQ THz, a été développé et optimisé. Des sources d'impulsions THz (antennes photoconductrices) ont été réalisées pour ce système permettant d'accéder à une large bande spectrale. Puis, ce système a été employé pour accéder au spectre du gain de LCQ THz, un paramètre clé, et en particulier appliqué à l'étude de LCQ hétérogènes (i.e. comprenant plus d'une région active permettant une émission large bande). Ces études ont permis de déterminer les facteurs limitant et d'améliorer leurs dessins, conduisant à un gain large et une émission laser à deux fréquences simultanément. En n, les propriétés non-linéaires résonantes de LCQ THz ont été étudiées. Une exaltation de la susceptibilité nonlin éaire a été démontrée en accordant un faisceau proche-IR avec des transitions interbandes du LCQ. En combinant cela à la grande puissance THz intracavité des LCQ, la conversion de l'émission THz du LCQ sur une porteuse optique proche-IR est montrée avec des e cacités élevées (0.12 %).

We introduce an approach to implement full coherent control on nanometer length scales. It is based on spatiotemporal modulation of the surface plasmon polariton (SPP) fields at the thick edge of a nanowedge. The SPP wavepackets propagating toward the sharp edge of this nanowedge are compressed and adiabatically concentrated at a nanofocus, forming an ultrashort pulse of local fields. The profile of the focused waveform as a function of time and one spatial dimension is completely coherently controlled. We establish the principal limits for the nanoconcentration of the terahertz (THz) radiation in metal/dielectric waveguides and determine their optimum shapes required for this nanoconcentration. We predict that the adiabatic compression of THz radiation from the initial spot size of vacuum wavelength R λ 300 μm 0 0 ≈ ≈ to the unprecedented final size of R = 100 − 250 nm can be achieved, while the THz radiation intensity is increased by a factor of 10 to 250. This THz energy nanoconcentration will not only improve the spatial resolution and increase the signal/noise ratio for THz imaging and spectroscopy, but in combination with the recently developed sources of powerful THz pulses, will allow the observation of nonlinear THz effects and a variety of nonlinear spectroscopies (such as two-dimensional spectroscopy), which are highly informative. This should find a wide spectrum of applications in science, engineering, biomedical research and environmental monitoring. We also develop a theory of the spoof plasmons propagating at the interface between a dielectric and a real conductor. The deviation from a perfect conductor is introduced through a finite skin depth. The possibilities of guiding and focusing of spoof plasmons are considered. Geometrical parameters of the structure are found which provide a good guiding of such modes. Moreover, the limit on the concentration by means of planar spoof plasmons in case of non-ideal metal is established. These properties of spoof plasmons are of great interest for THz technology.

We introduce an approach to implement full coherent control on nanometer length scales. It is based on spatiotemporal modulation of the surface plasmon polariton (SPP) fields at the thick edge of a nanowedge. The SPP wavepackets propagating toward the sharp edge of this nanowedge are compressed and adiabatically concentrated at a nanofocus, forming an ultrashort pulse of local fields. The profile of the focused waveform as a function of time and one spatial dimension is completely coherently controlled. We establish the principal limits for the nanoconcentration of the terahertz (THz) radiation in metal/dielectric waveguides and determine their optimum shapes required for this nanoconcentration. We predict that the adiabatic compression of THz radiation from the initial spot size of vacuum wavelength ~300 μm to the unprecedented final size of 100-250 nm can be achieved, while the THz radiation intensity is increased by a factor of 10 to 250. This THz energy nanoconcentration will not only improve the spatial resolution and increase the signal/noise ratio for THz imaging and spectroscopy, but in combination with the recently developed sources of powerful THz pulses, will allow the observation of nonlinear THz effects and a variety of nonlinear spectroscopies (such as two-dimensional spectroscopy), which are highly informative. This should find a wide spectrum of applications in science, engineering, biomedical research and environmental monitoring. We also develop a theory of the spoof plasmons propagating at the interface between a dielectric and a real conductor. The deviation from a perfect conductor is introduced through a finite skin depth. The possibilities of guiding and focusing of spoof plasmons are considered. Geometrical parameters of the structure are found which provide a good guiding of such modes. Moreover, the limit on the concentration by means of planar spoof plasmons in case of non-ideal metal is established. These properties of spoof plasmons are of great interest for THz technology.

In this thesis, the tunneling between individual atomic layers in structures of Bi2Sr2CaCu2O8+x based high-temperature superconductors are experimentally studied employing the intrinsic Josephson effect. A special attention is paid to the fabrication of small mesa structures using micro and nanofabrication techniques. In the first part of the thesis, the periodic Fraunhofer-like modulation of the critical current of the junctions as a function of in-plane magnetic field is investigated. A transition from a modulation with a half flux quantum to a flux quantum periodicity is demonstrated with increasing field and decreasing junction length. It is interpreted in terms of the transformation of the static fluxon lattice of stacked, strongly coupled intrinsic Josephson junctions and compared with theoretical predictions. A fluxon phase diagram is constructed.Numerical simulations have been carried out to complement the experimental data. In the second part of the thesis, different resonant phenomena are studied in the dynamic flux-flow state at high magnetic fields, including Eck-resonances and Fiske steps. Different resonant modes and their velocities, including superluminal modes, are identified. In the third part, different experiments attempting to detect radiation from small mesa structures using different setups based on hot-electron bolometer mixers and calorimeters are described. No distinct radiation with emission powers higher than about 500pW could be detected. Furthermore, the interaction with external GHz-radiation is studied. Resonances attributed to an induced flux-flow are observed, and the reflectivity of the sample can be tuned by switching mesas between the superconducting and quasiparticle state. In the last part, the resistive switching of mesas at high bias is studied. It is attributed to a persistent electrical doping of the crystal. Superconducting properties such as the critical current and temperature and the tunneling spectra are analyzed at different doping states of the same sample. The dynamics of the doping is studied, and attributed to two mechanisms; a charge-transfer effect and oxygen reordering

Le but de cette thèse est la synthèse optique d'ondes millimétriques et submillimétriques avec un très bas bruit de phase. La première partie concerne la réalisation d'un laser biaxe bifréquence dont chacune des deux fréquences est accordable indépendamment et continûment sur 1 THz. Ce laser est caractérisé en bruit d'amplitude et de phase. Nous avons mis en évidence un facteur de couplage entre les fluctuations de puissance de la diode de pompe et le bruit de phase du laser. La deuxième partie concerne le développement d'un système amplificateur qui se compose d'un amplificateur EDFA et d'un SOA par polarisation. Ce système amplificateur permet d'obtenir une puissance de l'ordre de 17 dBm, tout en réduisant le bruit relatif d'intensité (RIN) d'une vingtaine de dB sur 1 GHz. Cet amplificateur est également un actionneur pour la stabilisation de puissance permettant un RIN de l'ordre de -150 dB/Hz de 3 Hz à 5 kHz. La dernière partie concerne la mise en place du banc cavité et de l'asservissement des fréquences du laser sur une cavité ultra-stable. Nous obtenons un bruit de phase, à 10 kHz pour une porteuse à 10 GHz, meilleur que le plancher de bruit d'un analyseur de bruit de phase hautes performances de l'ordre de -115 dBc/ Hz. Le bruit de phase du système est indépendant de la fréquence de battement. / The aim of this thesis is the optical synthesis of millimeter and submillimeter waves with a very low phase noise. The first part concerns the development of a dual-axis dual frequency laser, whose the two frequencies are tuneable independently and continuously on 1 THz. This laser is characterized in amplitude noise and phase noise. We have identified a coupling factor between the diode pump and the power fluctuations of the laser phase noise. In the second part, we report the development of an amplifier system which consists of an EDFA and a SOA per polarisation axis. This amplifier system delivers 17 dBm of power and reduces the relative intensity noise (RIN) by 20 dB on a 1 GHz bandwidth. This amplifier is also an actuator for the power stabilization to a RIN of the order of -150 dB/Hz from 3 Hz to 5 kHz. The last part concerns the setup of the cavity bench and the stabilization of the laser frequency on a ultrastable cavity. We obtain a phase noise at 10 kHz of frequency offset on a 10 GHz carrier better than the noise floor of a phase noise analyser with high performance of the order of -115 dBc/Hz. The system phase noise is independent of the beatnote frequency.

The Quantum Cascade Laser (QCL)-based terahertz-over-fibre (ToF) concept combines the strength of QCLs as ultra-wide bandwidth, high speed data sources, with the mature optical fibre technology. In this thesis, for the first time, by fusing multiple technologies, digitally selected, electronically-switchable ToF concept is experimentally demonstrated. Furthermore, the digital mode selection principle and electronic tuning mechanism provided by novel aperiodic distributed feedback (ADFB) multi-band filters are presented. For the development of electronically tunable ADFB lasers, a range of bound-to-continuum and chirped superlattice terahertz (THz) QCLs are measured across the frequency range 2.9 – 4.5 THz. The availability of these active materials allowed rapid assessments of the optimum design parameters for subsequent measurements. First, a range of photonic lattice-engineered lasers operating at 4.4 THz are characterized and key design parameters identified. Following this initial development, full electrical and spectral characterization of ADFB lasers operating at 2.9 THz are presented. The novelty of this work lies in the first-ever successful demonstration of discretely tunable QCLs, operating at six distinct THz frequencies. The ADFB technology was experimentally applied using various device geometries and gain dynamics. Toward this aim, results are presented for a Y coupled QCL architecture, showing that complex on-chip signal manipulation can be extended into the THz regime. In addition, it is demonstrated that ADFB technology provides broadband multi-channel optical filtering for the entire gain bandwidth. It is shown that discrete, purely electronic, tuning of simultaneous dual colour output can be achieved. Multi band optical filter functions derived from ADFB gratings possess highly nonlinear dispersion across the filter bandwidth and are found to modify the gain-induced, driving current-dependent continuous mode tuning. This thesis, therefore, presents a systematic experimental analysis of the dispersion engineered continuous fine-tuning in THz QCLs. In the final two chapters, the thesis presents, for the first time, transmission of tunable THz signals over standard single-mode optical fibre by up converting 2.9 THz QCL radiation via intra-cavity nonlinear mixing with an optical fibre-injected near-infrared (NIR) carrier in the 1.3 µm band. Discrete and continuous tuning technologies, as developed in chapters 3 – 5, are now successfully transferred to THz sidebands on the NIR carrier, extracted via a butt coupled single mode fibre and recorded using an optical spectrum analyzer. The major novel outcome of this thesis is the first demonstration of electronically tunable phase-matched points in a THz plasmon waveguide. The key breakthrough is the experimental confirmation of the photonic band-gap engineering of group velocity of THz signals – as both ‘fast’ and ‘slow’ switchable side bands are observed. Such novel nonlinear up-conversion of spectrally flexible THz signals may open up new possibilities for ultrafast THz telecom frameworks.

京都大学 / 0048 / 新制・課程博士 / 博士(エネルギー科学) / 甲第22090号 / エネ博第398号 / 新制||エネ||76(附属図書館) / 京都大学大学院エネルギー科学研究科エネルギー応用科学専攻 / (主査)教授 大垣 英明, 教授 松田 一成, 教授 白井 康之 / 学位規則第4条第1項該当 / Doctor of Energy Science / Kyoto University / DFAM

京都大学 / 0048 / 新制・課程博士 / 博士(ｴﾈﾙｷﾞｰ科学) / 甲第20776号 / エネ博第361号 / 新制||エネ||71(附属図書館) / 京都大学大学院エネルギー科学研究科エネルギー応用科学専攻 / (主査)教授 大垣 英明, 教授 松田 一成, 教授 白井 康之 / 学位規則第4条第1項該当 / Doctor of Energy Science / Kyoto University / DFAM