The ever-increasing bandwidth requirements to support telecommunications infrastructure necessitates large-scale fabrication of low-cost and scalable silicon photonic integrated circuits. Wavelength-division multiplexing (WDM) schemes are fundamentally limited in the number of channels supported in long-haul transmission by the erbium doped fiber amplifier (EDFA). To address this, researchers have turned focus toward the thulium doped fiber amplifier (TDFA), which provides 3× more bandwidth. This thesis describes the development of high-speed silicon-on-insulator (SOI) micro-ring resonator (MRR) modulators optimized for wavelengths in the TDFA band. Chapter 2 presents a theoretical performance comparison between MRR modulators designed for optimized use at EDFA and TDFA wavelengths. Chapter 3 presents an experimental study of optical loss mechanisms at extended wavelengths which suggests reduced waveguide scattering and enhanced divacancy defect absorption as well as larger bending and substrate leakage losses when compared with shorter wavelengths. An electronic variable optical attenuator is characterized in Chapter 4 to experimentally verify the predicted 1.7× TDFA-band free-carrier effect enhancement over EDFA-band wavelengths. The first steady-state operation of an MMR modulator near a central wavelength of 1.97 µm is also demonstrated under the enhanced free-carrier effect. Chapter 5 demonstrates the first high-speed reverse bias operation of an MRR modulator with a measured bandwidth of 12.5 GHz, and an on-chip optical link consisting of a modulator followed by a defectmediated detector with open eye-diagrams up to data rates of 12.5 Gbps. Chapter 6 introduces an electrically-driven post-fabrication defect-assisted resonance trimming technique via local annealing for use in MRR devices. Chapter 7 presents a Monte Carlo simulation of resonance alignment in multi-MRR systems subjected to spatially-correlated wafer variation created through the Virtual Wafer Model process to predict thermal power consumption and power reduction through resonance trimming. / Thesis / Doctor of Philosophy (PhD)

Mid-infrared spectroscopic imaging, which leverages the inherent vibrational contrast of chemical bonds, has been a powerful analytical tool for sample characterization. However, its use in studying living systems is limited by low spatial resolution and significant water absorption. Recently developed mid-infrared photothermal (MIP) microscopy addresses these limitations by probing the absorption-induced photothermal effect using visible light. MIP microscopy achieves sub-micrometer spatial resolution and reduces water background interference. Yet, the imaging speed of current MIP microscopy is constrained by the challenge of measuring a small modulation over the probe laser background. This low imaging throughput hinders the visualization of living dynamics, and the rich molecular information in the spectroscopic domain is obscured due to the slow acquisition process. This dissertation explores solutions for enhancing imaging speed and spectral throughput and extending MIP imaging into visualizing chemical dynamics in living systems. In the first part of the dissertation, the mid-infrared photothermal process is studied and modeled in the time, frequency, and spatial domains using heat transfer analysis. Photothermal dynamics imaging (PDI) is introduced with the ability to visualize nanosecond-scale thermodynamics in samples upon laser excitation. By capturing all higher-order harmonics, PDI achieves more than a four-fold improvement in signal-to-noise ratio compared to the lock-in method for detecting low-duty cycle photothermal signals. An imaging speed nearly two orders of magnitude faster than the lock-in counterpart has been reached. In addition, PDI captures the transient thermal field evolution, providing a tool to gauge the target’s physical properties and microenvironment. In the second part, a video-rate MIP microscope is introduced based on the PDI detection method. In the system, a synchronized IR and visible beam scanning scheme is developed, enabling photothermal detection with a single IR pulse at each pixel. Moreover, synchronized laser scanning allows uniform MIP imaging in a field of view over hundreds of micrometers while maintaining a high spatial resolution. This capability enabled the visualization of fast chemical dynamics inside living fungal cells, cancer cells, and living worms, providing an imaging platform for biology research. Having reached the speed limitation of single-pulse imaging, we further advanced the speed of spectroscopic imaging by moving beyond the conventional measurement of absorption contrast in the photothermal process. In the final part of this dissertation, we revisited the photothermal process from the perspective of energy deposition, discovering that the absorption coefficient is reflected in the slope of the heating process rather than its overall amplitude. We demonstrated mid-infrared energy deposition (MIRED) spectroscopy using a 32-channel quantum cascade laser array that emits a broadband pulse train in microseconds. With MIRED, we achieved hyperspectral mid-infrared imaging on a microsecond scale.

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Cette thèse est dédiée à l’étude de la génération de supercontinuum (SCG) deforte puissance moyenne dans le domaine spectral entre 2 mm et 5,5 mm. Un laser à fibredopée thulium (Tm3+) opérant dans un régime simultanément déclenché et à verrouillage demodes (QML) a été développé. En régime continu ce laser a délivré 70 W et en régime QML,26Wmoyens ont été obtenus pour des taux de répétition en QS de 180 kHz ou plus. L’énergiela plus élevée contenue dans une enveloppe QS a été évaluée à 166 mJ avec 66 mJ contenuedans la sous-impulsion à verrouillage de mode la plus énergétique. L’émission du laser àfibre correspondait toujours à un facteur de qualité M2 excellent, entre 1,1 et 1,2. La SCGcouvrant la plage spectrale de 2 mm à 5,5 mm a été réalisée en implémentant différentes fibresen cascade. Des supercontinua jusqu’à environ 4 mm ont été générés dans des fibres en fluorurepuis pour la plage spectrale complémentaire entre 4 mm et 5,5 mm, des fibres en chalcogénureont été utilisées.La puissance moyenne maximale de 7,8 W a été démontrée pour un supercontinuum dans unefibre en ZBLAN. Le spectre s’étend jusqu’à 4,2 mm. Au total, 69%/43%/30%/16,5% de lapuissance totale ont été mesurés au-delà de 2,15 mm/2,65 mm/3,1 mm/3,5 mm respectivement.La fibre en InF3 a permis d’atteindre une puissance moyenne de 0,8 W et le supercontinuums’étend jusqu’à 2,95 mm.Pour les essais d’élargissement spectral complémentaire, trois fibres en chalcogénure ont étéutilisées. L’élargissement spectral a été démontré pour toutes les fibres en chalcogénure.Jusqu’à 20 mW de puissance ont été obtenus avec une fibre As2Se3. Le spectre a été étendujusqu’à 4,9 mm. / This thesis reports about the investigation of high power supercontinuum (SC)generation between 2 mm and 5.5 mm. A Q-switched mode-locked (QML) thulium (Tm3+)-doped fiber laser has been developped to pump different nonlinear fibers. The fiber laserprovided in continuous wave regime an output power of 70 W. In QML operation, 26 W havebeen obtained with Q-switched repetition rates of 180 kHz or higher. The highest energy of theQS envelopes has been 166 mJ with 66 mJ contained in the most-energetic ML pulses, whichhave been surrounded by Gaussian-like pedestals with temporal widths around 2.5 ns. On topof these pedestals, very short temporal peaks with pulse durations around 15 ps appeared. Thehighest achieved peak power of a pedestal has been 25 kW. The beam parameter product M2of the fiber laser has been measured in different operational regimes and resulted always in anexcellent value around 1.2.The highest SC output power level from a ZBLAN fiber has been 7.8 W. In total, 69%/43%/30%/16.5% of the transmitted SC output radiation could be converted beyond the wavelengthof 2.15 mm/2.65 mm/3.1 mm/3.5 mm, respectively, with the broadest output spectrum from theZBLAN fiber exceeding 4.2 mm. The InF3 fiber provided a total output power of 0.8 W withan output spectrum up to 2.95 mm.Successful broadening of the wavelength-limited SC output from the ZBLAN fibers has beenachieved with all three investigated chalcogenide fibers with as much as 20 mW of outputpower by using an arsenic selenide fiber. The output spectrum exceeded 4.9 mm.

<p>Infrared absorption spectra can provide analytically useful information on a large variety of compounds, ranging from small ions to large biological molecules. In fact, all analytes that possess a dipole moment that changes during vibration are infrared-active. The infrared (IR) spectrum can be subdivided into far-, mid- and near- regions. The focus of attention in this thesis is the mid-IR region, in which the fundamental vibrations of most organic compounds are located, thus providing scope for positive structural identification. However, while such near-ubiquitous signals can be very useful for monitoring simple molecules in simple systems, they can be increasingly disadvantageous as the number of analytes and/or the complexity of the sample matrix increases. Thus, hyphenation to a separation system prior to detection is desirable. Paper I appended to this thesis presents (for the first time) the on-line hyphenation between Fourier transform infrared spectroscopy, FTIR, and capillary zone electrophoresis, CZE. CZE is a highly efficient separation technique that separates ionic analytes with respect to their charge-to-size ratio. It is most commonly performed in aqueous buffers in fused silica capillaries. Since these capillaries absorb virtually all infrared light an IR-transparent flow cell had to be developed. In further studies (Paper II) the applicability of CZE is expanded to include neutral analytes by the addition of micelles to the buffer, and micellar electrokinetic chromatography, MEKC, was successfully hyphenated to FTIR for the first time. Paper III describes an application of the on-line CZE-FTIR technique in which non-UV-absorbing analytes in a complex matrix were separated, identified and quantified in one run.</p><p>Measuring aqueous solutions in the mid-IR region is not straightforward since water absorbs intensely in this region, sometimes completely, leaving no transmitted, detectable light. For this reason, quantum cascade lasers are interesting. These lasers represent a new type of mid-IR semiconducting lasers with high output power due to their ingenious design. The laser action lies within one conduction band (intersubband) and can be tailored to emit light in the entire mid-IR region using the same semiconducting material. To investigate their potential to increase the optical path length in aqueous solutions, these lasers were used with an aqueous flow system (Paper IV), and the experience gained in these experiments enabled hyphenation of such lasers to a CZE system (Paper V).</p>

Infrared absorption spectra can provide analytically useful information on a large variety of compounds, ranging from small ions to large biological molecules. In fact, all analytes that possess a dipole moment that changes during vibration are infrared-active. The infrared (IR) spectrum can be subdivided into far-, mid- and near- regions. The focus of attention in this thesis is the mid-IR region, in which the fundamental vibrations of most organic compounds are located, thus providing scope for positive structural identification. However, while such near-ubiquitous signals can be very useful for monitoring simple molecules in simple systems, they can be increasingly disadvantageous as the number of analytes and/or the complexity of the sample matrix increases. Thus, hyphenation to a separation system prior to detection is desirable. Paper I appended to this thesis presents (for the first time) the on-line hyphenation between Fourier transform infrared spectroscopy, FTIR, and capillary zone electrophoresis, CZE. CZE is a highly efficient separation technique that separates ionic analytes with respect to their charge-to-size ratio. It is most commonly performed in aqueous buffers in fused silica capillaries. Since these capillaries absorb virtually all infrared light an IR-transparent flow cell had to be developed. In further studies (Paper II) the applicability of CZE is expanded to include neutral analytes by the addition of micelles to the buffer, and micellar electrokinetic chromatography, MEKC, was successfully hyphenated to FTIR for the first time. Paper III describes an application of the on-line CZE-FTIR technique in which non-UV-absorbing analytes in a complex matrix were separated, identified and quantified in one run. Measuring aqueous solutions in the mid-IR region is not straightforward since water absorbs intensely in this region, sometimes completely, leaving no transmitted, detectable light. For this reason, quantum cascade lasers are interesting. These lasers represent a new type of mid-IR semiconducting lasers with high output power due to their ingenious design. The laser action lies within one conduction band (intersubband) and can be tailored to emit light in the entire mid-IR region using the same semiconducting material. To investigate their potential to increase the optical path length in aqueous solutions, these lasers were used with an aqueous flow system (Paper IV), and the experience gained in these experiments enabled hyphenation of such lasers to a CZE system (Paper V).

Nonlinearities in quantum cascade lasers (QCL¡¯s) have wide applications in wavelength tunability and ultra-short pulse generation. In this thesis, optical nonlinearities in InGaAs/AlInAs-based mid-infrared (MIR) QCL¡¯s with quadruple resonant levels are investigated. Design optimization for the second-harmonic generation (SHG) of the device is presented. Performance characteristics associated with the third-order nonlinearities are also analyzed. The design optimization for SHG efficiency is obtained utilizing techniques from supersymmetric quantum mechanics (SUSYQM) with both material-dependent effective mass and band nonparabolicity. Current flow and power output of the structure are analyzed by self-consistently solving rate equations for the carriers and photons. Nonunity pumping efficiency from one period of the QCL to the next is taken into account by including all relevant electron-electron (e-e) and longitudinal (LO) phonon scattering mechanisms between the injector/collector and active regions. Two-photon absorption processes are analyzed for the resonant cascading triple levels designed for enhancing SHG. Both sequential and simultaneous two-photon absorption processes are included in the rate-equation model. The current output characteristics for both the original and optimized structures are analyzed and compared. Stronger resonant tunneling in the optimized structure is manifested by enhanced negative differential resistance. Current-dependent linear optical output power is derived based on the steady-state photon populations in the active region. The second-harmonic (SH) power is derived from the Maxwell equations with the phase mismatch included. Due to stronger coupling between lasing levels, the optimized structure has both higher linear and nonlinear output powers. Phase mismatch effects are significant for both structures leading to a substantial reduction of the linear-to-nonlinear conversion efficiency. The optimized structure can be fabricated through digitally grading the submonolayer alloys by molecular beam epitaxy (MBE). In addition to the second-order nonlinearity, performance characteristics brought by the third-order nonlinearities are also discussed, which include third-harmonic generation (THG) and intensity dependent (Kerr) refractive index. Linear to third-harmonic (TH) conversion efficiency is evaluated based on the phase-mismatched condition. The enhanced self-mode-locking (SML) effect over a typical three-level laser is predicted, which will stimulate further investigations of pulse duration shortening by structures with multiple harmonic levels.

<p>This thesis discusses a new scheme for generating radiation in the mid infrared spectral region, especially the 3.5-5 µm range. The scheme uses established Nd³⁺-lasers at 1.06 µm and down conversion in nonlinear optical crystals. The down conversion is made by two optical parametric oscillators (OPO) in series. The second OPO is a classical OPO using a zink germanium phosphide (ZGP) crystal. ZGP is the best nonlinear material available for the 4-8 µm spectral range, but it is absorbing below 2 µm. The new development presented in this thesis is the OPO used to convert the 1.06 µm laser radiation to a suitable OPO pump near 2 µm.</p><p>The OPO uses a type I quasi phase-matched crystal, which accesses high nonlinearities and avoids walk-off. The problem with type I OPOs close to degeneracy is the broad bandwidth of the generated radiation, which reduces the efficiency of a second OPO. This has been solved with a spectrally selective cavity using a volume Bragg grating output coupler. Unlike other bandwidth limiting schemes this introduces no intracavity losses and thus efficient OPO operation is achievable.</p><p>Narrow linewidth (~0.5 nm) OPO operation has been achieved with periodically poled LiNbO₃ (PPLN) and periodically poled KTiOPO4 (PPKTP) while locking the signal wavelength at 2008 nm and simultaneously generating an idler at 2264 nm. A high average power PPLN OPO with 36 % conversion efficiency and 47 % slope efficiency is reported. Operation very close to degeneracy at 2128 nm with the narrowband signal and idler peaks separated by 0.6 nm was demonstrated in a PPKTP OPO. Both the signal at 2008 nm and the combined signal and idler around 2128 nm from the PPKTP OPOs have been used to show efficient pumping of a ZGP OPO. The maximum conversion efficiency from 1 µm to the mid-IR demonstrated is 7 % with a slope efficiency of 10 %. This is not quite as high as what has been presented by other authors, but the experiments reported here have not shown the optimum efficiency of the new scheme. Relatively simple improvements are expected to give a significant increase in conversion efficiency.</p>

Mid-infrared (IR) lasers (2-12 μm) have found tremendous applications in medical surgeries, spectroscopy, remote sensing, etc. Nowadays, mid-IR emissions are usually generated from semiconductor lasers, gas lasers, and solid-state lasers based on nonlinear wavelength conversion. However, they usually have disadvantages including poor beam quality, low efficiency, and complicated configurations. Mid-IR fiber lasers have the advantages of excellent beam quality, high efficiency, inherent simplicity, compactness, and outstanding heat-dissipating capability, and have attracted significant interest in recent years. In this dissertation, I have studied and investigated Q-switched and mode-locked fiber lasers in the mid-IR wavelength region. My dissertation includes six chapters: In Chapter 1, I review the background of mid-IR lasers and address my motivation on the research of mid-IR fiber lasers; In Chapter 2, I present the experimental results of microsecond and nanosecond Er³⁺-doped and Ho³⁺-doped fiber lasers in the 3 μm wavelength region Q-switched by Fe²⁺:ZnSe and graphene saturable absorbers. In Chapter 3, Q-switched 3 μm laser fiber amplifiers are investigated experimentally and theoretically and their power scaling are discussed. In Chapter 4, a graphene mode-locked Er³⁺-doped fiber lasers at 2.8 μm with a pulse width < 50 ps is presented. In Chapter 5, extending the spectral range of mid-IR fiber lasers by use of nonlinear wavelength conversion is addressed and discussed. I have proposed 10-watt-level 3-5 μm Raman lasers using tellurite fibers as the nonlinear gain medium and pumped by our Er³⁺-doped fiber lasers at 2.8 μm. In the last chapter, the prospect of mid-IR fiber laser is addressed and further research work is discussed.

This thesis focuses on the utilisation of mid-infrared techniques in technological atmospheric pressure, non-thermal plasma (NTP) diagnostics. Two mid-infrared techniques were demonstrated in this work namely laser absorption and Fourier transform infrared (FTIR) spectroscopy. The performance of external-cavity quantum cascade laser (EC-QCL), a relatively new laser type with broad tuning capability was also demonstrated as potential diagnostics tool for technological NTP applications. A dual plate dielectric barrier discharge (DBD) and a packed-bed NTP reactor were designed and fabricated to perform plasma process. Quantitative analysis of the laser absorption and FTIR spectroscopy techniques for gas detection were validated by using standard gas samples. Real-time CO monitoring by means of in-situ laser absorption spectroscopy measurements were performed for gas phase diagnostics in the decomposition of TEOS by means of plasma-enhanced chemical vapour deposition (PE-CVD) and in CO2 reforming of CH4 by means of NTP. In-line FTIR measurements simultaneously recorded the gas spectrum at the exhaust of the plasma reactors. Information from both measurements was found to provide useful information on the plasma processes and chemistry for the NTP applications. Finally, wavelength stability and linearity performance of a broad tuning range EC-QCL were evaluated by using the Allan variance technique. (LOD) at SNR = 1 was estimated to be ~ 2 ppm, achieved under atmospheric pressure, at the room temperature, and a path length of 41 cm for NO detection produced from the decomposition of dichloromethane (DCM) by means of NTP.