Terahertz (THz) frequency range (wavelength of 300-30 μm, frequency of 1-10 THz and photon energy of ~4-40meV), the gap between infrared and microwave electromagnetic waves, have remained relatively unexplored for a long time, due to lack of a high power, coherent, and compact source, as well as the lack of an appropriate detector and the transmission devices. THz wave has recently received considerable attention for potential applications in non-invasive medical imaging, detecting trace of gases in the environment, sensing of organic and biological molecules, security controls, local oscillators for heterodyne receiver systems, free space communication, etc. THz quantum cascade laser (QCL), as the relatively high power and coherent THz radiation source, was demonstrated in 2002. After near a decade of intense research, THz QCLs operate only up to 186K in pulse mode with maximum power of 250 mW at 10 K. This thesis discusses many aspects of theoretical and experimental design considerations for THz QCLs. The objective is to obtain a laser device that emits high powers and works towards the temperatures achievable by thermoelectric coolers. This work includes designing the active gain medium, and the engineering of the waveguide and heat removal structures. A density matrix based model is developed to explain the charge transport and gain mechanism in the intersubband devices, particularly for three well resonant phonon based THz QCLs. The model allows for designing of the optimum and novel active gain mediums that work at higher temperatures. The designed active gain mediums are fabricated using discussed low loss waveguide and efficient heat removal structures. The maximum operating temperatures as high as ~176 K is achieved. Finally a promising lasing scheme based on phonon-photon-phonon emissions is proposed that improves the population inversion and offers high gain peak.

Terahertz (THz) frequency range (wavelength of 300-30 μm, frequency of 1-10 THz and photon energy of ~4-40meV), the gap between infrared and microwave electromagnetic waves, have remained relatively unexplored for a long time, due to lack of a high power, coherent, and compact source, as well as the lack of an appropriate detector and the transmission devices. THz wave has recently received considerable attention for potential applications in non-invasive medical imaging, detecting trace of gases in the environment, sensing of organic and biological molecules, security controls, local oscillators for heterodyne receiver systems, free space communication, etc. THz quantum cascade laser (QCL), as the relatively high power and coherent THz radiation source, was demonstrated in 2002. After near a decade of intense research, THz QCLs operate only up to 186K in pulse mode with maximum power of 250 mW at 10 K. This thesis discusses many aspects of theoretical and experimental design considerations for THz QCLs. The objective is to obtain a laser device that emits high powers and works towards the temperatures achievable by thermoelectric coolers. This work includes designing the active gain medium, and the engineering of the waveguide and heat removal structures. A density matrix based model is developed to explain the charge transport and gain mechanism in the intersubband devices, particularly for three well resonant phonon based THz QCLs. The model allows for designing of the optimum and novel active gain mediums that work at higher temperatures. The designed active gain mediums are fabricated using discussed low loss waveguide and efficient heat removal structures. The maximum operating temperatures as high as ~176 K is achieved. Finally a promising lasing scheme based on phonon-photon-phonon emissions is proposed that improves the population inversion and offers high gain peak.

This thesis focuses on addressing some important aspects of the life cycle of interstellar clouds through observational submillimeter and millimeter-wave studies of star formation and molecular cloud environments and the development of instrumentation to enable these studies.We examine the influence of star formation on parent molecular clouds through a case study of protostellar sources in the Mon OB1 northern cloud complex. An energetics analysis of these star forming regions and associated molecular outflows was carried out, suggesting that the cloud complex maintains its overall integrity, except along outflow axes and that the coupling between outflow kinetic energy and cloud turbulent energy is weak, < ~0.5%. In order to study the larger picture of cloud formation and disruption, this work was expanded to explore the molecular environment at cloud boundaries. To this end, acloud edge survey was undertaken consisting of multi-transition strip scan observations of CO and 13CO toward molecular clouds with a broad range of stellar and star forming characteristics. Our work supports the interpretation that cloud formation is taking place along the southeastern edge of Heiles Cloud 2, and the results will be used as a framework for guiding the analysis of other surveyed cloud edges.Achieving observational capabilities enabling effective studies of life cycles of the ISM is becoming possible through a new generation of heterodyne spectroscopic instruments. Here, we report on characterization measurements of a prototype mixer unit for the 64-pixel SuperCam array, an instrument commissioned to mapover 500 square degrees of the Galactic Plane with very high resolution at 345 GHz. These measurements were crucial to verifying the overall array design and anticipating its performance. Spectroscopic capabilities at THz (< 300 microns) frequencies permits access to a host of diagnostic tools (e.g., high-J CO, CI, NII, & CII) uniquely suited to probe crucial properties of the ISM. The development of heterodynetechnology at these frequencies is largely limited by availability of compact, powerful sources of local oscillator power. We explore the use of waveguide spatial filters in conjunction with Quantum Cascade Lasers, a promising power source at frequenciesabove ~ 2 THz.

The extension of Multi-mode Absorption Spectroscopy (MUMAS) to the infra-red spectral region for multi-species gas sensing is reported. A computationally efficient, theoretical model for analysis of MUMAS spectra is presented that avoids approximations used in previous work and treats arbitrary and time-dependent spectral intensity envelopes, thus facilitating the use of commercially available Interband Cascade Lasers (ICLs) and Quantum Cascade Lasers (QCLs). The first use of an ICL for MUMAS is reported using a multi-mode device operating at 3.7 &mu;m to detect CH₄ transitions over a range of 30 nm. Mode-linewidths are measured using the pressure-dependent widths of an isolated absorption feature in HCl. Multi- species sensing is demonstrated by measurement of partial pressures of CH₄, C₂H₂ and H₂CO in a low-pressure mixture with uncertainties of around 10&percnt;. Detection of CH₄ in N₂ at 1 bar is demonstrated using a shorter-cavity ICL to resolve spectral features in pressure-broadened and congested spectra. The first use of a QCL for MUMAS is reported using a commercially available device operating at 5.3 &mu;m to detect multiple absorption transitions of NO at a partial pressure of 2.79 &mu;bar in N₂ buffer gas. The revised model is shown to enable good fits to MUMAS data by accounting for the time-variation of the spectral intensity profile during frequency scanning. Individual mode-linewidths are derived from fits to pressure- dependent MUMAS spectra and features from background interferences due to H₂O in laboratory air are distinguished from those of the target species, NO. Data obtained at scan rates up to 10 kHz demonstrate the potential for achieving short measurement times. The development of a balanced ratiometric detection scheme for MUMAS with commercially available multi-mode lasers operating at 1.5 &mu;m is reported for simultaneous detection of CO and CO₂ showing improved SNR performance over previous direct transmission methods and suitability for a compact field-employable instrument. In addition, MUMAS spectra of CO₂ are used to derive gas temperatures with an uncertainty of 3.2&percnt; in the range 300 - 700 K.

Application of InAs/AlSb materials system for development of short-wavelength quantum cascade lasers is explored. Molecular beam epitaxy (MBE) technology allowing to grow multiperiodical unstrained InAs/AlSb heterostructures with roughness of 1-2 monolayers is developed. It is demonstrated that InAs/AlSb materials system is well-suitable for development of short-wavelength quantum cascade lasers operating below 4 µm wavelength. Lasers containing plasmon-enhanced waveguides as well as the short period InAs/AlSb superlattices as waveguides were designed, MBE-grown and studied. The effect of waveguide properties on the device parameters is revealed. Usage of these waveguides and innovations in laser active region introducing “funnel” injector allowed one to reach operation temperature 420 K at the emission wavelength of 3.3 µm. The obtained optical peak power exceeded 1 W per facet. The room temperature operation has been obtained at wavelength below 3 µm. As for wavelength range, applying the new active region design strategy and the short period InAs/AlSb superlattice spacers InAs based quantum cascade lasers emitting at the wavelengths as short as 2.63 µm were developed, which is today the shortest emission wavelength of the operation of semiconductor lasers based on the intersubband transitions. / Disertaciniame darbe nagrinėjamas InAs/AlSb medžiagų sistemos panaudojimas trumpabangių tarppajuostinių lazerių kūrimui. Buvo išplėtota molekulinių pluoštelių epitaksijos technologija, leidžianti auginti daugiaperiodines neįtemptas InAs/AlSb heterosandūras su mažu 1-2 atominių sluoksnių šiurkštumu. Buvo parodyta, jog InAs/AlSb medžiagų sistema yra tinkama kurti trumpabangiams kvantiniams kaskadiniams lazeriams, veikiantiems žemiau 4 µm bangos ilgio ribos. Buvo ištirtas kvantinių kaskadinių lazerių, turinčių tiek plazmoninius bangolaidžius su stipriai legiruotais InAs apdariniais sluoksniais, tiek ir mažo periodo InAs/AlSb supergardelių bangolaidžius, veikimas bei jų įtaka prietaiso parametrams. Šie sprendimai dėl bangolaidžių bei tolimesni aktyviosios terpės patobulinimai, naudojant piltuvėlio formos injektorių, leido sukurti didelio našumo prietaisus, galinčius veikti iki 420 K temperatūros, esant 3,3 µm bangos ilgio emisijai, ir pasiekti maksimalią optinę galią siekiančią 1 W kambario temperatūroje. Šios inovacijos leido sukurti ir InAs/AlSb kvantinį kaskadinį lazerį, emituojantį ~2,6 µm bangos ilgio spinduliuotę  šiai dienai tai yra trumpiausią bangos ilgį spinduliuojantis tokio tipo prietaisas pasaulyje.

Disertaciniame darbe nagrinėjamas InAs/AlSb medžiagų sistemos panaudojimas trumpabangių tarppajuostinių lazerių kūrimui. Buvo išplėtota molekulinių pluoštelių epitaksijos technologija, leidžianti auginti daugiaperiodines neįtemptas InAs/AlSb heterosandūras su mažu 1-2 atominių sluoksnių šiurkštumu. Buvo parodyta, jog InAs/AlSb medžiagų sistema yra tinkama kurti trumpabangiams kvantiniams kaskadiniams lazeriams, veikiantiems žemiau 4 µm bangos ilgio ribos. Buvo ištirtas kvantinių kaskadinių lazerių, turinčių tiek plazmoninius bangolaidžius su stipriai legiruotais InAs apdariniais sluoksniais, tiek ir mažo periodo InAs/AlSb supergardelių bangolaidžius, veikimas bei jų įtaka prietaiso parametrams. Šie sprendimai dėl bangolaidžių bei tolimesni aktyviosios terpės patobulinimai, naudojant piltuvėlio formos injektorių, leido sukurti didelio našumo prietaisus, galinčius veikti iki 420 K temperatūros, esant 3,3 µm bangos ilgio emisijai, ir pasiekti maksimalią optinę galią siekiančią 1 W kambario temperatūroje. Šios inovacijos leido sukurti ir InAs/AlSb kvantinį kaskadinį lazerį, emituojantį ~2,6 µm bangos ilgio spinduliuotę  šiai dienai tai yra trumpiausią bangos ilgį spinduliuojantis tokio tipo prietaisas pasaulyje. / Application of InAs/AlSb materials system for development of short-wavelength quantum cascade lasers is explored. Molecular beam epitaxy (MBE) technology allowing to grow multiperiodical unstrained InAs/AlSb heterostructures with roughness of 1-2 monolayers is developed. It is demonstrated that InAs/AlSb materials system is well-suitable for development of short-wavelength quantum cascade lasers operating below 4 µm wavelength. Lasers containing plasmon-enhanced waveguides as well as the short period InAs/AlSb superlattices as waveguides were designed, MBE-grown and studied. The effect of waveguide properties on the device parameters is revealed. Usage of these waveguides and innovations in laser active region introducing “funnel” injector allowed one to reach operation temperature 420 K at the emission wavelength of 3.3 µm. The obtained optical peak power exceeded 1 W per facet. The room temperature operation has been obtained at wavelength below 3 µm. As for wavelength range, applying the new active region design strategy and the short period InAs/AlSb superlattice spacers InAs based quantum cascade lasers emitting at the wavelengths as short as 2.63 µm were developed, which is today the shortest emission wavelength of the operation of semiconductor lasers based on the intersubband transitions.

Les lasers à  cascade quantique (QCLs) sont des sources laser à  semi-conducteurs permettant de fortes puissances optiques dans le moyen-infrarouge. Les applications visées sont la spectroscopie à  distance et les contre-mesures optiques. Les performances des QCLs restent limitées par le transport électronique, le comportement optique et la dissipation de la charge thermique. Premièrement, cette thèse a permis une meilleure compréhension des éléments limitants les performances des QCLs. Les propriétés optiques et thermiques des matériaux qui constituent les QCLs ont été mesurées. En nous appuyant sur des simulations, nous avons montré l'impact de la géométrie du composant et de l'embase sur les performances. Deuxièmement, nous avons étudié des méthodes pour mettre en forme le faisceau afin d'augmenter la luminance du QCL. Nous avons ainsi montré que le couplage avec des fibres optiques ou l'utilisation de QCLs à  section évasée permettent de réduire la divergence du QCL. De plus, nous avons obtenu de très fortes puissances crêtes et moyennes avec des lasers larges tout en conservant un bon champ lointain. Enfin, nous avons montré qu'il est possible de mettre en forme le faisceau émis par des QCLs larges en réinjectant le signal optique. Dernièrement, nous avons proposé des nouvelles méthodes pour réaliser des réseaux de QCLs couplés monolithiquement. En plus de résultats expérimentaux sur des réseaux de QCLs uniformes, nous avons montré les limites des réseaux non-uniformes. Enfin, nous avons breveté une solution basée sur des antiguides en silicium amorphe pour coupler un grand nombre de QCLs. / Quantum cascade lasers (QCLs) are semiconductor laser sources able to produce high output power in mid-infrared range. Target applications are remote spectroscopy and optical counter-measure. Their performances are still limited by electronic transport, optical behavior and thermal load dissipation. First, this work has lead to a better comprehension of the features limiting the QCLs performances. Optical and thermal properties of the materials the QCLs are made of have been measured. By simulation, we have shown the impact of the device and submount's geometries on the performances. Second, we have studied some methods to shape the beam in order to increase the luminance of the QCL. We have then demonstrated that coupling with optic fibers, or using tapered QCLs reduces the divergence of the QCL. In addition, we have obtained very high peak and average powers with broad area (BA) QCLs, while keeping a good far-field quality. Finally, we have shown that it is possible to shape the beam emitted by BA QCLs by optical feedback. Lastly, we have proposed new methods to conceive monolithically phase-locked QCL arrays. On top of experimental results on uniform QCL arrays, we have shown the limits of non-uniform arrays. Finally, we have patented a solution based on amorphous silicon antiguides to phase-lock a large number of QCLs.

In several fields, such as biology, chemistry, combustion and environmental science, laser absorption spectroscopy represents an invaluable tool for the detection and identification of a variety of molecular species in the gas phase. For this detection to be quantitative, it is of paramount importance to rely on accurate spectroscopic parameters for the involved absorption lines in terms of line strength, line center frequency, pressure broadening, and pressure shift coefficients. The mid-infrared region offers the most favorable conditions for sensitive and chemically selective detection. The sensitivity derives from the presence of intense fundamental ro-vibrational transitions of molecules, whereas chemical selectivity relates to the unique absorption spectrum that molecules possess in the mid-IR region, thereby known as the fingerprint region. In this thesis, we combine the accelerating technology of optical frequency combs (OFC), which are powerful tools for accurate optical frequency measurements, with the wide tunability and single line emission in the mid-IR of extended cavity quantum cascade lasers (EC-QCL), to perform highly resolved, accurate and sensitive measurements in the fingerprint region, from 7.25 to 8 μm. Specifically, we have been able to lock for the first time the optical frequency of an EC-QCL to an OFC by utilizing nonlinear optics in the form of sum frequency generation (SFG) (Lamperti, AlSaif et al., 2018) and have exploited this comb-locked EC-QCL for an accurate survey of the entire ν1 ro-vibrational band of one of the most important greenhouse gases, nitrous oxide (N2O). The developed spectrometer is able to operate over a wide region of ~ 100 cm-1, in a fully automated fashion, while affording a 63 kHz uncertainty on the retrieved line center frequencies. The measurement allowed us to determine very accurately rotational constants of both ground and excited states of the ν1 band of N2O through the measurements of tens of lines of the P and R branches (AlSaif et al., JQSRT 2018). The spectrometer was then upgraded with a more recent and narrower linewidth EC-QCL to perform sub-Doppler saturated spectroscopy on the same N2O sample at a spectral resolution below 1 MHz, the sharpest ever observed with this type of laser. Finally, we worked at adding high sensitivity to the apparatus by introducing the gas in a high-finesse passive resonator and by developing a system to measure the intra-cavity absorption with cavity ring-down spectroscopy (CRDS) together with comb calibration.

Alors que l'étude de l'atmosphère a une importance croissante pour répondre aux problématiques environnementales, les exigences en terme de sources laser pour la spectrométrie de molécules complexes nécessitent de développer des sources largement accordables. Le travail de thèse présenté dans ce manuscrit est centré sur la mise en œuvre de lasers à cascade quantique en cavité étendue (EC-QCL). Une partie de ce travail concerne la caractérisation d'une source EC-QCL commerciale ainsi que son application à la détection de gaz par spectrométrie photoacoustique. Des mesures ont été réalisées sur le dioxyde de carbone dans l'air expiré et sur le butane. La partie centrale de ce travail de thèse réside dans le développement de sources EC-QCL à partir de puces laser à cascade quantique développées par le III-V Lab. L'objectif est d'obtenir des sources largement accordables qui puissent être utilisées pour la détection de molécules complexes. Cela comprend la simulation, la conception et la mise en œuvre de systèmes en cavité étendue. Deux sources EC-QCL ont été réalisées. La première est une source impulsionnelle émettant autour de 4,5μm. La seconde émet autour de 7,5μm et fonctionne en continu à température ambiante. Ce laser a été utilisé pour réaliser des enregistrements sur l'acétone et le trichlorure de phosphoryle. / As the study of the atmosphere is growing strongly in response to environmental issues, the needs in terms of laser sources for spectroscopy of complex molecules require the development of widely tunable sources. The PhD work presented in this manuscript is focused on the implementation of quantum cascade lasers in external cavity (EC-QCL). Part of this work deals with the characterization of a commercial EC-QCL source and its application to gas detection by photoacoustic spectrometry. Measurements were performed on carbon dioxide in exhaled air and butane. The central part of this thesis consists in the development of ECQCL sources based on quantum cascade laser chips from III-V Lab. The aim is to obtain widely tunable sources that can be used for the detection of complex molecules. This includes simulation, design and implementation of external cavity systems. Two EC-QCL sources were implemented. The first one is a pulsed laser emitting around 4,5μm. The second one emits around 7,5μm and is operated at room temperature in continuous wave mode. This laser was used to record the spectra of acetone and phosphoryl chloride.

Au cours des dix dernières années, les performances des lasers à cascade quantique dans le moyen infrarouge ont connu une progression rapide: Les rendements ont atteint des valeurs supérieures à 20% avec une puissance d’émission de 5W en régime continu, à température ambiante. Ces valeurs ont été atteintes notamment grâce à la diminution de la sensibilité des lasers à l’échauffement, avec des températures caractéristiques T0 s’approchant de 300K. Les performances sont donc actuellement limitées par la puissance injectée, qui est proportionnelle à la taille de la zone de gain. Les travaux de cette thèse présentent une solution innovante, consistant à combiner un réseau d’émetteurs de petites tailles de façon monolithique. Nous démontrons expérimentalement pour la première fois, des dispositifs jusqu’à 32 émetteurs de 2µm de larges, émettant en phase par couplage évanescent. De plus, nous mettons en évidences des résistances thermiques record. Ces résultats mettent en évidence la possibilité de fabriquer des sources de hautes puissances (supérieures à 10W) dans le moyen-infrarouge avec une très bonne qualité de faisceau. / During the last 10 years, the quantum cascade lasers performances in the mid-infrared have been considerably improved: the wall plug efficiency has reached values superior to 20%, with output power up to 5W in continuous wave operation, at room temperature. Those values have been achieved due to the reduction of the temperature sensibility of the lasers, with characteristic temperature T0 reaching 300K. The output power is now limited to the injected power, which is proportional to the gain region size. This thesis reports an innovating solution consisting on beam combining an array of narrow emitters, monolithically. We experimentally demonstrate for the first time devices of up to 32 emitters of 2µm width emitting in phase by evanescent coupling. Moreover, we show record thermal resistance. Those results highlight the possibility to fabricate high power sources (superior to 10 W) in the mid-infrared, with a good beam quality.