Dissertations / Theses on the topic 'Optical parametric oscillators'

This thesis describes the design and implementation of several novel, nanosecond pulsed, intracavity optical parametric oscillators for the generation of terahertz radiation. The application of the intracavity approach in the context of terahertz optical parametric oscillators has been demonstrated for the first time, and the pump wave energy required was thereby reduced by an order of magnitude. The terahertz wave was tunable from under 1THz up to 3THz with a free running linewidth of ~50GHz and pulse energies up to ~20nJ (pulses were a few nanoseconds in duration). The terahertz beam profile was of Gaussian shape and could be focussed down to 2.3 times the diffraction limited spot size (M² values of 2.3 and 6.7 in the components of the beam parallel and perpendicular to the silicon prism array output coupler respectively). Developments of this intracavity source with regard to the linewidth are also reported. Implementation of etalons in the optical (laser and OPO) cavities was shown to be a promising technique that brings the terahertz linewidth down below 1GHz (close to the transform limit of nanosecond pulses) while retaining the tuning range and beam characteristics of the free running system. Close to Fourier transform limited pulses were obtained (<100MHz linewidth) via an injection seeding technique, although with significantly increased system complexity. A deleterious effect caused by the mode beating of a multimode host laser was also discovered, in that sidebands were induced on the seeded downconverted wave. This has wider implications in the field of intracavity OPOs. Finally, quasi-phasematching techniques implementing periodically poled lithium niobate were investigated as a way to lower the downconversion threshold energy requirement (by collinear propagation of the optical waves), and also to extract the terahertz wave rapidly from the (highly absorbing in the terahertz region) lithium niobate crystal. The existence of two phasematching solutions arising from the bidirectionality of the grating vector was identified as a serious design constraint in the context of an OPO where either solution can build up from noise photons, and so prefers the solution with the lowest walkoff of the downconverted waves - possibly resulting in unextractable terahertz radiation. Quasi-phasematching with an orthogonal grating vector (with identical but opposite phasematching solutions) was demonstrated and cascaded downconversion processes observed and characterised. These cascaded processes are permitted by the collinearality of the optical waves and may allow efficiency improvements through overcoming the quantum defect limit. This research has resulted in four peer reviewed papers in respected journals, and the intracavity terahertz OPO has been licensed to a company who have commercialised the technology (M Squared Lasers, Glasgow).

The all-solid-state (or "holosteric") optical parametric oscillator has resulted from the recent development of diode-laser-pumped solid-state lasers and from recent advancements in new optically nonlinear materials. As a result, all-solid-state sources of widely tunable (ultraviolet - visible - near infrared) coherent radiation are now possible by using the radiation from diode-laser-pumped solid-state lasers, either directly or after frequency conversion, to pump optical parametric oscillators. Such devices can be made compact, efficient and reliable. The work described in this thesis explores the feasibility of obtaining widely tunable radiation from such devices, with particular reference to low threshold, high efficiency operation, so requiring only modest energies (1 mJ in ultraviolet) from the pump source. In particular, a frequency tripled or frequency quadruped Nd:YAG laser pumped by pulsed, GaAlAs diode laser bars has been used as the pump source, and lithium triborate has been used as the nonlinear medium in the optical parametric oscillator. Two geometries of lithium triborate crystals have been investigated as the nonlinear medium. One was cut for a type II non-critical phase matching geometry, while the other was cut for a type I critical phase matching geometry. The oscillator cavities were designed for optimum focusing and mode matching aiming for operation with a low pump energy through the use of tightly focused pump radiation. The ultraviolet pump source was based on a Q-switched diode-laser-pumped Nd:YAG laser which generated pulses at 1.064 mum with energy 10 mJ and duration around 10 ns. These were then frequency up-converted to the UV at 355 nm or 266 nm, so as to be suitable for pumping the parametric oscillators. Generally, an overall conversion efficiency from 1.064 mum to 355 nm of >30% was obtained using the nonlinear materials potassium titanyl phosphate and lithium triborate for second harmonic generation and sum-frequency mixing respectively. For conversion to 266 nm, an overall efficiency of > 18 % was obtained using the nonlinear materials KTP and BBO for two step second harmonic generation. In the experimental investigations of the all-solid-state lithium triborate optical parametric oscillator pumped at 355 nm a low oscillation threshold was obtained in the type II non-critical phase matching geometry (around 0.2 mJ) and pump depletions of 50 % were obtained at around six times threshold. This device could be temperature tuned (20 - 200 &deg;C) from 457 to 481 nm (signal wave) and 1.6 to 1.35 mum (idler wave). Optimised focusing conditions corresponding to the theory of Guha et al were approached in the type I phase matching geometry, and despite the existence of a 1&deg; walkoff angle, the minimum oscillation threshold was measured to be around 0.3 mJ. Generally, pump depletions of about 35 % were obtained, at around four times threshold. These devices could be angle tuned (through crystal internal angle 14&deg;) from 457 to 666 nm (signal wave) and 1.6 mum to 768 nm (idler wave). (The whole of the range 420 nm to 2.3 mum could be covered with such a device given additional mirror sets). The all-solid-state type II geometry lithium triborate optical parametric oscillator was also pumped at 266 nm, when it was temperature tunable (20 - 200 &deg;C) from 306 to 314 nm (signal wave) and 2.03 to 1.75 mum (idler wave). Pump depletions of 25 % were demonstrated with this device at pump energies of four times threshold. In addition to the above experimental investigations, the thesis addresses the issues of (i) choice of nonlinear material for optical parametric oscillators in terms of appropriate figures of merit, and (ii) optimisation of pump and resonated wave focusing parameters. Reviews of the appropriate theoretical background to phase matching geometries and optical parametric interaction are included.

This thesis describes the development of a new generation of pulsed optical parametric oscillators (OPO's) based on two new non-linear materials, urea and beta-BaB2O4 (or BBO), and pumped by a new class of laser pump sources, namely, excimer lasers, to provide broadly tunable coherent radiation in new regions of the electromagnetic spectrum, particularly in the ultraviolet and the visible, which have previously been inaccessible. The laser pump source used during this work was a pulsed ultraviolet XeCl excimer laser operating at 308nm. Because of the stringent demands on the pump beam quality (with regard to both spatial and spectral coherence) for successful operation of OPO's, the pump laser was designed and constructed as an injection-seeded system, to provide a narrow-linewidth, near-diffraction-limited output beam, with sufficiently high peak powers to enable OPO operation. In this way, we were able to obtain an output beam with a linewidth &le; 0.2cm-1, and a full-angle of divergence as low as 60muR (~3 times the diffraction limit). The maximum energy available from the pump laser was 30mJ, in pulses measuring typically 10ns in duration. The output beam was also linearly polarised to better than 95%, and the pulse repetition rate was 1 Hz. In the early part of this work, we used the constructed pump laser to investigate spontaneous parametric fluorescence in a home-grown urea sample, in order to characterise the crystal, and to compare the observed spectrum with the calculated OPO tuning curves. The results of these experiments were found to be in good agreement with the theoretical predictions. The main thrust of the project, however, was the development of an OPO based on urea as the non-linear medium and pumped at 308nm by the narrowband XeCl excimer laser. We were successful in constructing such an OPO, using an 8-mm-long, home-grown crystal, and were able to generate, continuously tunable output from 572 to 667nm, with a 2.5% energy conversion efficiency. The timing range of the device was later extended to 537-720nm, by utilising a 15-mm-long, home-grown urea sample, and its conversion efficiency was improved to as high as 37% at 90&deg; phase-matching, with &ge; 10% efficiency over a 100-nm range in the visible (from 570 to 670nm). Finally, in an effort to achieve even higher efficiencies, we performed experiments in a 25-mm-long commercial urea crystal, and demonstrated exceptionally high external energy conversion efficiencies of up to 66%, with evidence of even higher levels of pump depletion (as high as 85%) at 90&deg; phase-matching. The latter part of the project was concerned with the design and development of a similar device based on the new non-linear material, beta-BaB2O4, to provide continuously tunable radiation over a much broader tuning range, particularly in the blue and the near ultraviolet, not accessed by the urea OPO. We used a 12-mm-long commercially available beta-BaB2O4 crystal to construct this OPO, and successfully operated this device over the entire wavelength range from 354nm in the near ultraviolet, throughout the visible, to 2.37mum in the near infrared, with an energy conversion efficiency in excess of 10% over the range 450-960 nm. The constructed OPO's were also characterised with regard to several operating parameters, including oscillation threshold, spectral linewidth, as well as spatial and temporal variation and, where appropriate, the experimental results were compared with the predictions of theory.

A low threshold, efficient optical parametric oscillator (OPO) based on the material Potassium Titanyl Phosphate (KTP) and pumped by a diode-laser-pumped, Q-switched Nd:YLF laser has been demonstrated and investigated. This all-solid-state device was operated in a non-critical phase match (NCPM) geometry converting the 1 mum pump light to output wavelengths of 1.54 and 3.28 mum, and has potential as an 'eyesafe' laser source with scaling to higher powers. A major contributing factor to the success of this work was the extension of the steady state theory of the singly resonant OPO to include the build-up time effects that are dominant in the pulsed regime. A number of diode pumped lasers were constructed, allowing a comparison to be made between side- and end-pumping geometries, and also between the materials Nd:YAG and Nd:YLF. The end-pumping geometry in conjunction with the higher absorption and longer upper state lifetime in Nd:YLF made it the design of choice for the case of low pump pulse energies (~ 12 mJ at 797 nm). Anamorphic expansion of the laser mode in the plane parallel to the diode laser junction was employed to achieve TEM00 operation of this laser. Subsequent Q-switching with a polariser and LiNbO3 Pockels cell combination produced 2.2 mJ at 1.047 mum in an 18 ns pulse. Investigation of the dynamic loss of the Q-switch (which is due to the elasto-optic effect) allowed improvement of laser performance. The established model for a pulsed singly resonant OPO which describes the case for a plane-plane resonator was inappropriate in this work and so the steady state focused beam theory was extended to include time dependence. Fair agreement was found between the computer model and the experimental results, where the effects of pump and signal focusing, and output coupling were investigated. The high conversion efficiency of 30% for converting the 1 mum pump light to the eyesafe wavelength of 1.54 mum is superior to the present alternative source of the Er:glass laser. Pump energy thresholds of less than 0.5 mJ were obtained, along with internal conversions approaching 50 %. An empirical relation describing pump depletion was derived which showed good agreement with experiment. A high resolution investigation of the spectral properties of the OPO identified the roles of resonant reflection and doubly resonant behaviour on the mode structure of the output. The former suggests a way in which single mode operation could be achieved without the use of additional intracavity elements, or a seeding source.

The work described in this thesis is concerned with the development of self-modelocked Ti:sapphire lasers and femtosecond optical parametric oscillators based on periodically-poled rubidium titanyl arsenate and periodically-poled lithium niobate and operating in the near and mid-infrared. In Chapter 1 the theory of ultrashort pulse generation is explained with regard to the Ti:sapphire laser. The optical properties of Ti:sapphire are discussed along with the principles of laser oscillation and pulse generation. The techniques used to modelock the lasers used in the experimental work, which follows, are also considered. The second part of the chapter deals with typical measurement techniques for characterising femtosecond optical pulses from a laser or an OPO, including a detailed explanation of second harmonic generation autocorrelation. Chapter 1 concludes with a thorough description of frequency-resolved optical gating, the newest of these pulse characterisation techniques. In Chapter 2 the subject of nonlinear optics and the properties of nonlinear optical materials are discussed. Phasematching in nonlinear optical materials is explained along with the principle techniques for achieving this, including birefringent phasematching and quasi-phasematching. A review of techniques for periodically- poling nonlinear optical crystals is also given. The chapter concludes with a section on the optical effects of group velocity dispersion and self-phase modulation, that influence the output from an ultrashort pulse laser or OPO and describes methods for second and third-order dispersion compensation. Chapter 2 concludes the theory required to explain the experiments described in Chapters 3, 4, 5 and 6. Chapter 3 describes the operation and characterisation of two different Ti:sapphire laser systems involving different methods of dispersion compensation. The first laser produces 100 fs duration self-modelocked laser pulses and dispersion compensation is achieved by including a pair of prisms in the cavity. This laser system is discussed further in Chapter 5, where it is operated in conjunction with a Spectra Physics Millennia, as the pump source for an all-solid-state femtosecond OPO based on periodically-poled lithium niobate. A second laser system is described in Chapter 3, which produces self-modelocked pulses of ~15 fs duration and dispersion compensation is achieved by including chirped multilayer dielectric mirrors in the cavity. The subject matter that Chapter 4 is concerned with includes the operation and characterisation of a femtosecond OPO based on PPRTA. Ti:sapphire pump wavelength tuning and cavity-length tuning of the OPO are shown to produce wavelengths throughout the range 1.060 mum to 1.225 mum in the signal and 2.67 jam to 4.5 mum in the idler, with average output powers as high as 120 mW in the signal and 105 mW in the idler output. The effects of photorefractive damage are minimal and consequently this offers the possibility of room-temperature operation of the PPRTA- based OPO. Chapter 5 is concerned with the generation of longer idler wavelengths, in the region of 5 mum, from an all-solid-state OPO based on periodically-poled lithium niobate. The approach used with the PPRTA-based OPO is extended to PPLN and in Chapter 5, results are presented which show that the use of an all-solid-state Ti:sapphire pump source in combination with a PPLN-based OPO represents a robust source of high- repetition-rate femtosecond pulses in the mid-infrared at wavelengths out to ~5 mum. Significantly higher output powers in the signal and idler than previously reported are also measured. In Chapter 6 a similar PPLN-based OPO is described, with modifications to the cavity elements, to reduce the output pulse duration of the OPO. This system is pumped by a sub- 20 fs Ti:sapphire laser. A pulse duration of 175 fs is recorded for the signal at a wavelength of 1.07 mum. Output powers of 28 mW for the signal at 1.07 mum and 6.8 mW for the idler at 2.7 mum are also measured. The tuning range for the signal extends from 1.045 mum to 1.190 mum, and for the idler, extends from 2.57 mum to 3.67 mum.

The research presented in this thesis is concerned with the generation and characterisation of femtosecond pulses in the near and mid-infrared spectral regions. The three optical parametric oscillators which were constructed were synchronously- pumped by a self-modelocked femtosecond Ti:sapphire laser. Noncollinear critical birefringent phasematching was used in an oscillator based on KTiOAsO4, which was tunable from 1.03 to 1.2 mum and 2.51 to 4.1 mum by varying the crystal angle. The mid-infrared pulses were sub-100 fs, and essentially free from frequency chirp. With appropriate dispersion compensation the near-infrared signal pulses were temporally compressed to 69 fs. Theoretical models of noncollinear phasematching were derived and the results agreed closely with experiment. A novel optical parametric oscillator design based on a semi-monolithic noncritically phasematched RbTiOAsO4 crystal was implemented. This unique cavity configuration allowed independent focussing of the pump and signal beams within the crystal. It facilitated a reduction in cavity length to bring the signal pulse repetition rate into synchronism with the second (172 MHz) and fourth (344 MHz) harmonics of the pump pulse repetition frequency. Extraction efficiencies as high as 55% were observed. Quasi-phasematched femtosecond optical parametric oscillation was demonstrated in periodically poled lithium niobate. This device offered extensive tunability, covering 0.975 to 1.54 mum in the signal branch and 1.67 to 4.55 mum in the idler branch, from a combination of grating, pump wavelength and cavity length tuning. A theoretical model indicated that a very broad gain bandwidth allowed the wide tuning range. An attractively low oscillation threshold of 45 mW was recorded, and a visible output of 70 mW at 540 nm was observed, caused by simultaneously phasematched frequency-doubling of the signal output. The pulses from the Ti:sapphire laser and from the optical parametric oscillators were characterised by autocorrelation and frequency-resolved optical gating techniques. A highly advantageous autocorrelator arrangement based on quadratic nonlinearity in light-emitting diodes and photodiodes was demonstrated, and a novel second harmonic generation frequency-resolved optical gating system allowed real-time monitoring of pulsed outputs and complete characterisation of the intensity and phase of pulses.

High-repetition-rate femtosecond laser sources are essential laboratory tools for spectroscopy, microscopy, amongst other applications. With the relative length of one femtosecond to one second being similar to the length of 1 second compared to the age of the universe, such lasers enable scientists to probe physical processes at unimaginably short timescales. Furthermore, the high peak powers can excite strong nonlinear response in delicate material samples without delivering potentially damaging levels of energy. The infrared (IR) spectral region across 1–12 μmis rich in molecular absorption features, but in general poorly served by conventional coherent light sources. Optical parametric oscillators (OPOs) represent the most viable solution to this long-term issue, due to their table-top nature, and unparalleled tunability and spectral brightness in the near- and mid-IR. Recent breakthroughs in nonlinear crystal technology have opened the door to the generation of laser light in the previously difficult to access region above 4 μm, using high power lasers near 1 μm. Exploiting these new nonlinear materials to improve the spectral coverage and output power of OPOs has the potential to provide important societal benefits, particularly in the fields of frequency metrology, security, and medical imaging. In addition, theoretical modelling and exploration of devices with novel cavity designs can lead to technological advances which improve OPO affordability and increase their appeal to a wider scientific audience. In this thesis, we have demonstrated three OPOs across 1–8.4 μm in the infrared, which are pumped using well-established Ti:sapphire laser technology. The first is a compact and cost-effective device tunable across 1051–1700 nm in the near-IR, producing sub-100 fs pulses at 80 MHz. The incorportion of an optical fibre into the cavity leads to excellent passive power and wavelength stability, and enables soliton formation to be observed, together with other interesting nonlinear effects. We have also demonstrated an efficient, low-threshold mid-IR OPO exploiting group-velocity match effects in MgO:PPLN, which enables the use of a long (42 mm) nonlinear crystal. In doing so, we report quantum conversion efficiencies as high as 48% from the near-IR (s1 μm) pump to the mid-IR (3.1–4.3 μm), and use the source to perform basic spectroscopy. The third device uses Ti:sapphire light at s1 μm to directly pump the new nonlinear crystal, CdSiP2, generating up to 20 mW average power across 6.6–8.4 μm in the deep mid-IR. As the first demonstration of a single-stage Ti:sapphire-pumped deep mid-IR OPO with practical output powers, it has potential for medical imaging applications in the important amide II and III regions. Finally, upconversion imaging using femtosecond OPOs is reported and briefly discussed, together with future directions for deep mid-IR generation using orientationpatterned gallium phosphide (OP-GaP)<br>Las fuentes de láser de femtosegundo son instrumentos esenciales para espectroscopia, microscopía, entre otras aplicaciones. Dado que la duración relativa de un femtosegundo a un segundo es comparable con la duración de 1 segundo con respecto a la edad del universo, estos láseres permiten a los científicos investigar procesos físicos en escalas de tiempo increíblemente cortas. Además, las altas potencias de pico pueden provocar fuertes respuestas no lineales en materiales delicados sin entregar niveles de energía potencialmente dañinos. La región espectral del infrarrojo (IR) tiene numerosas características de absorción molecular, pero en general está mal servida por fuentes de luz coherentes convencionales. Los osciladores ópticos paramétricos (OPOs) representan la solución más viable para este problema a largo plazo, debido a su portabilidad, su capacidad de sintonizar y brillo espectral en el IR cercano y medio. Los avances recientes en la tecnología de cristales no lineales han permitido la generación de luz en la región de difícil acceso inferior a 4 μm, utilizando láseres de alta potencia cercanos a 1 μm. La explotación de estos nuevos materiales no lineales para mejorar la cobertura espectral y la potencia de salida de los OPOs, tiene el potencial de ofrecer beneficios sociales importantes, especialmente a través de los campos de metrología de frecuencias, seguridad e imágenes médicas. Además, el modelado teórico y la exploración de dispositivos con diseños de cavidades novedosos, puede conducir a avances tecnológicos que mejoran la asequibilidad del OPO y aumentan su atractivo para una audiencia científica más amplia. En esta tesis, hemos demostrado tres OPO en el rango espectral de 1–8.4 μm en el infrarrojo, que se bombean utilizando tecnología de làser bien establecida como el Ti: sapphire. En primer lugar, se demostró un dispositivo compacto y rentable, sintonizable a través de 1051–1700 nm en el IR cercano, que produce pulsos <100 fs a 80 MHz. La incorporación de una fibra óptica en la cavidad conduce a una excelente potencia pasiva y estabilidad de la longitud de onda, y permite observar la formación de solitones, con otros efectos no lineales interesantes. También hemos demostrado un OPO de infrarrojo medio eficiente, de bajo umbral, que explota la coincidencia de velocidad de grupo en MgO:PPLN, que permite el uso de un cristal no lineal largo (42 mm). Al hacerlo, reportamos eficiencias de conversión cuántica tan altas como 48% desde la bomba de IR cercano (~ 1 μm) hasta el IR medio (3.1–4.3 μm), y usamos la fuente para realizar la espectroscopia básica. El tercer dispositivo utiliza luz de láser Ti:sapphire cerca de 1 μm para bombear directamente el nuevo cristal no lineal CdSiP2, generando hasta 20 mW de potencia promedio con longitud de onda de 6.6–8.4 μm en el IR medio profundo. Como la primera demostración de un OPO de infrarrojo medio bombeado por un Ti:sapphire láser en una sola etapa con potencias de salida prácticas, tiene potencial para aplicaciones de imágenes médicas en las importantes regiones amida II y III. Finalmente, las imágenes de conversión ascendente que utilizan un OPO de femtosegundo es comentada y analizada brevemente, junto con los futuros avances para la generación de IR profundo con un cristal de OP-GaP.

A study of new materials for optical parametric oscillators (OPOs) was carried out using an XeCI excimer laser as a pump source. The three non-linear optical materials studied were lithium borate (LBO), deuterated L-arginine phosphate (d-LAP) and β-barium borate (BBO). These optical parametric oscillators were characterised for oscillation thresholds, tuning ranges, linewidths and efficiencies. A novel device in LBO was demonstrated, using the non-critically phase matched type II geometry. The device displayed a low oscillation threshold, which was independent of pump beam area thus made it attractive for use with low energy pump sources. The device was also shown to have a narrow inherent linewidth, oscillating on only one or two axial modes. Other geometries in LBO were also explored. The type I critical geometry displayed a very large tuning range covering the near ultra-violet, the visible and the near infra-red spectral regions. The type IT yz geometry was also studied. An OPO in d-LAP was demonstrated for the first time. The device was tunable in the blue/green spectral region and also in the near infra-red. A low threshold was observed for large beam sizes. Optically induced damage caused by the ultra-violet pump was also encountered. A comparison of the thresholds, efficiencies and tuning ranges of the three materials, LBO, d-LAP and BBO, was made and the suitability of each material for use in a line-narrowed oscillator discussed. Although possessing the largest linewidth, BBO was found to be the best suited due to its low oscillation threshold and large tunability. A single axial mode BBO OPO was demonstrated that was tunable from 385 nm to 560 nm and from 2300 nm to 684 nm. The line-narrowed OPO was then used for linewidth control of other devices. Firstly, an injection seeded OPO was demonstrated and the device was characterised for threshold and linewidth. Secondly, the line-narrowed OPO was used to seed an optical parametric amplifier (OPA). Single pass gains of ~20 were observed from the OPA.

<p>Optical parametric oscillators (OPOs) and optical parametricamplifiers (OPAs) constitute a class of optical frequencyconverting devices that have many possible applications, e.g.in range finding, molecular spectroscopy and medicine. They canconvert the frequency of the incident pump field with highefficiency, and generate two waves at new frequencies that willbe continuously tuneable over a wide spectral range. Virtuallyany wavelengths within the transparency region of the nonlinearmaterial can be generated if the material can bequasi-phasematched (QPM). In addition, QPM gives thepossibility to utilise the largest nonlinear tensor element ofthe material and allows walk-off free interaction between thewaves.</p><p>The aims of this thesis have been to investigate thepossibility to use QPM KTiOPO₄crystals as nonlinear material in nanosecond OPOsand OPAs operating at room-temperature, and to explore theadvantages and shortcomings of these devices. The technique ofelectric field poling has been employed to implement the QPMstructure in flux grown KTiOPO₄(KTP).</p><p>The main conclusion is that periodically poled KTP (PPKTP)is a suitable material to use in nanosecond OPOs and OPAs. Thematerial properties that foremost make KTP into an attractivenonlinear material are: The large value of the nonlinearcoefficient d₃₃, the high resistance to optically inducedbreakdown, the low susceptibility to grey-track formation, theinsensitivity to the photorefractive effect, the widetransparency and the low coercive field.</p><p>The thesis shows that it is possible to pole large volumesof KTP with a high quality of the QPM structure. Highlyefficient nanosecond OPOs have been constructed during thisproject. Maximum conversion efficiencies have reached 45 % inthe case of a singly resonant OPO (SRO) built around a 3 mmthick PPKTP crystal. Total pulse energies for both the signal(1.72 µm) and the idler (2.8 µm) of up to 18 mJ wasreached and an average output power of 2 W was obtained forthis sample. However, up to 24 W was produced in a doublyresonant OPO operating close to degeneracy. The efficiencyreached 48 % for that case. Truly continuous and very widespectral tuning has also been demonstrated, as well as a narrowbandwidth OPO operating on one single longitudinal mode.</p><p><b>Keywords:</b>optical parametric oscillators, opticalparametric amplifiers, quasi-phasematching, KTiOPO₄, nonlinear optics, frequency conversion, periodicelectric field poling, ferroelectrics, high-order secondharmonic generation, electro-optic effect.</p>

<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>

Several pulsed optical oscillators (OPOs) based on periodically poled lithium niobate (PPLN) and pumped by single longitudinal mode Ti:sapphire lasers have been developed. These OPOs provide access to important spectroscopic regions in the 1 - 5.5 [mu]m region and can be rapidly turned by varying the pump wavelength. Previously many of the OPOs developed to take advantage of PPLN relied on a combination of period selection and temperature tuning and as a result were slow and cumbersome to tune. This problem my be avoided by using tunable pump sources or acoustically induced strain waves. Several candidate OPO pump sources were characterised. These pump sources with themselves pumped by lasers operating at repetition reates of either 1.5 kHz (high repetition rate) or 10Hz (low repetition rate). High repetition rate systems include: a Ti-sapphire laser, injection seeded by a single longitudinal mode diode laser, several coupled cavity Ti:sapphire lasers with bandwidths less than 100 Ghz and Cr:forsterite lasers narrowed by prisms and étalons. The low repetition rate systems were all coupled cavity Ti:sapphire lasers one of which was single and double pass amplified. Of these it was found that only the high repetition rate injection seeded laser and the low repetition Ti:sapphire lasers were suitable as OPO pump sources. OPOs were characterised at high and low repetition rates. The high repetition rate system exhibited a low threshold of oscillation (18.7 [mu]J) and a low overall efficiency (25%) which was thought to be due to the pulse to pulse variability of the Ti:sapphire bandwidth. The tuning range of the OPO was 932 to 1310 nm (signal) and 1.989 [mu]m to 5.281 [mu]m (idler) using multiple poling periods and only 15 nm of pump tuning. OPO oscillation on two separate signals simultaneously was observed. Two separate low repetition rate systems were investigated; the first was tuned from 1200 to 1600 nm (signal) and from 1600 to 2400 nm (idler) on a single poling period with a high absolute efficiency of 35% and a threshold of 180 [mu]J. The second OPO was tuned from 940 to 1220 nm (signal) and 2.2 to 4.3 [mu]m (idler) on a single poling period. The absolute efficiency of the system was 25% and the threshold was 200 [mu]J. OPO oscillation on two separate signals was investigated using an OPO based on grazing incidence configured cavity. It was found that the signals coupled together through Raman transitions present in lithium niobate and that coupling reduced the efficiency of the device as a whole. The affect of an acoustically induced strain field on the optical nonlinearity of tetragonal ferroelectric materials was investigated. It was found that the optical nonlinear coefficient varies linearly with the cell displacement and as the square root of the acoustic power. A crystal designed to implement a quasi phase matched interaction based on this variation is proposed.

The purpose of this thesis was to investigate the possibilities of enhancing the temporal and spatial coherence of parametric devices in the mid-infrared spectrum by exploiting inherent coherence selection of Bessel beams. Several optical parametric oscillators (OPO) were constructed and characterized for various types of resonators and pump lasers. In the first part of this work an OPO was constructed out of a periodically poled KTP (PPKTP) crystal within a stable resonator. It was pumped by a Q-switched Nd:YAG laser in transversal and longitudinal single mode operation. The OPO was pumped at 1064 nm and operated at signal wavelength of 1595.9 nm with a bandwidth at FWHM of 0.2 nm and idler wavelength 3192.9 nm and bandwidth of 0.5nm at FWHM. The stable resonator was constructed out of a curved input coupler and a planar output coupler to generate a spatially coherent beam. The beam quality factor of the OPO was measured to M2=1.3 and M2=1.7 in the horizontal and the vertical direction respectively. In the second part of this work conical beams, and hence noncollinear phase matching, was used. This was done to improve and study the temporal and spatial coherence of the generated beam if the OPO is pumped by a laser operating in multiple transversal and longitudinal modes. Using noncollinear phase matching provides a possibility of generating a highly coherent signal (or idler) wave when using a pump laser which operates in multiple transversal and longitudinal modes. Usually, such pump laser makes it difficult to generate highly coherent beams since the properties, such as bandwidth and beam quality factor, of the pump laser are transferred to the generated waves. So called multimode lasers, which operate in multiple modes, can be considered inexpensive and reliable while providing high pulse energies, and they are therefore attractive as pump sources for nonlinear processes. Throughout this second part a Q-switched Nd:YAG laser operating in multiple transversal and longitudinal modes at a wavelength 1064 nm was used. Optical parametric generation (OPG) was used to compare the effects between pumping with a Gaussian wave, and collinear phase matching, and pumping with a conical, a Bessel beam and hence noncollinear phase matching. Thereafter, optical parametric oscillation was studied with collinear and noncollinear phase matching using a Fabry-Perot cavity. The OPO pumped by a Q-switched Gaussian beam, and hence using collinear phase matching had a signal wave at 1596.3 nm and a bandwidth at FWHM of 4 nm. The OPO pumped by a conical beam, hence a Bessel beam and noncollinear phase matching, had a signal wave at 1596.5 nm and a bandwidth at FWHM of 0.2 nm. Both OPOs had a beam quality factor M2~2 in horizontal and vertical direction.

In this thesis, we have demonstrated various ultrafast optical parametric oscillators (OPOs) based on different nonlinear media. The thesis consists of OPO systems, novel techniques, designs, and concepts that has facilitated the wavelength accessibility from 1 µm in the near-infrared region to as far as 8 µm in the mid-infrared region. We developed a fs OPO based on BiB3O6 (BIBO) directly pumped the Kerr-lens mode-locked (KLM) Ti:sapphire laser. This system could provide broad and rapid tuning from 1420-1560 nm just by changing the cavity length. Also, by exploiting the unique optical properties of BIBO under type I (e¿oo) interaction, we have demonstrated the first self-phase-locked degenerate fs OPO. Further, we have developed a technique called synchronous retro-reflection for threshold reduction and signal amplification before the onset of the oscillation. This technique is generic and is particularly useful while deploying ultrafast OPOs with birefringent materials that have relatively low nonlinear gain and when we have limited pump power. In addition, we have developed a dual-wavelength fs OPO with arbitrary and independent tuning by making use of anti-resonant-ring (ARR) or Sagnac interferometer. This universal technique of coupling two optical oscillators can be employed in any time regime (cw to ultrafast pico or fs) irrespective of the operating wavelengths. This conceptual technique can be used for intracavity terahertz (THz) generation which exploits the high intensity intracavity oscillating pulses. Also, we have developed a dual-crystal, double-pumped OPOs for intracavity signal amplification in fs regime as well as in ps regime, for arbitrary and independent wavelength tuning. In both systems two crystals share the same optical cavity but are pumped independently by a single laser source. Finally, we have devised and experimentally demonstrated a novel concept of pumping an OPO within another OPO using a composite cascaded cavity design. This all solid-state Ti:sapphire-pumped fs OPO system is potentially capable of providing access to mid-infrared region beyond 4 µm to as far as 18 µm by careful selection of the nonlinear medium.<br>En esta tesis, hemos demostrado varios osciladores ópticos paramétricos ultrarrápidos (OPO) basados en diferentes medios no lineales. La tesis consta de sistemas OPO, técnicas novedosas, diseños y conceptos que han facilitado el acceso a longitudes de onda de 1 μm en la región del infrarrojo cercano, así como hasta 8 μm en la región del infrarrojo medio. Hemos desarrollado un femtosegundo (fs) OPO basado en BiB3O6 (BIBO) directamente bombeado por un láser Kerr-lens mode-locked (KLM) de Ti:zafiro. Este sistema proporciona amplia y rápida sintonización en el rango 1400-1560 nm con sólo cambiar la longitud de la cavidad. También, gracias a las propiedades ópticas únicas de BIBO en la interacción tipo I (e-->oo), hemos demostrado el primer fs OPO self-phaselocked degenerado. Además, hemos desarrollado una técnica llamada retro reflexión sincronizada para la reducción del umbral y amplificación de señal, antes de la aparición de la oscilación. Esta técnica es genérica y es particularmente útil para implementar OPOs ultrarrápidos con materiales birrefringentes que tienen relativamente baja ganancia no lineal y cuando existe una limitación de la potencia de bombeo. Adicionalmente, hemos desarrollado un fs OPO con longitud de onda dual que presenta sintonización arbitraria e independiente mediante el uso de un interferómetro de anillo antirresonante (ARR) o Sagnac. Esta técnica universal de acoplamiento de dos osciladores ópticos puede ser empleada en cualquier régimen temporal (desde cw a ultrarrápido de pico o femtosegundo) e independientemente de las longitudes de onda de operación. Esta técnica puede ser utilizada para la generación de THz intracavidad, permitiendo aprovechar la alta intensidad de los pulsos oscilantes. Además, hemos desarrollado un sistema OPO de doble cristal y doble bombeo para la amplificación de la señal dentro de la cavidad tanto en régimen de fs como de ps, para el ajuste de longitud de onda arbitraria e independiente. En ambos sistemas los dos cristales comparten la misma cavidad óptica, pero son bombeados independientemente por una sola fuente láser. Por último, hemos diseñado y demostrado experimentalmente un concepto novedoso para bombear un OPO dentro de otro OPO mediante un diseño de cavidad compuesta en cascada. Este sistema de estado sólido OPO de femtosegundo bombeado por el láser de Ti: zafiro es potencialmente capaz de proporcionar acceso a la región del infrarrojo medio más allá de 4 μm incluso hasta las 18 μm, realizando una cuidadosa selección del medio no lineal

This thesis shows how sources of coherent radiation in the mid-infrared (mid-IR) region can be enhanced. To achieve this, optical parametric oscillators (OPOs) employing improved novel materials, new optical elements, and novel cavity designs have been implemented. Moreover, important measurements for the development of ultrashort-pulsed lasers were conducted. In turn, such lasers are suitable pump sources for the nonlinear conversion to the mid-IR. The mid-infrared spectral region is of interest for many applications in the areas of medicine, sensing, climate monitoring, and ranging. Here the target wavelength 6.45μm was especially interesting since it is considered particularly useful in surgical applications. Commercially available lasers perform poorly as pump sources for the generation of this wavelength. Therefore, a superior cascaded conversion scheme with large aperture crystals was implemented. In these, Rb-doped KTiOPO4(KTP) was employed since it was found that Rb-doping improves the poling properties of KTP. Moreover, for the conversion scheme to be efficient, a narrow-band out putspectrum of the OPO is required. It was shown here that this can successfully be achieved by utilizing a volume Bragg grating (VBG). Alternatively, for the direct generation of mid-IR radiation, KTiOAsO4(KTA) crystals with an extended transmission into the mid-IR as compared to KTP have been investigated. Novel room-temperature periodic-poling of KTA was shown and the fabricated crystals were successfully employed in a highly-efficient OPO. The newly developed pump sources based on the Rb-doped KTP crystals were successfully implemented in a cascaded OPO experiment. Here, a so-called RISTRA cavity was employed and high-energy nanosecond pulses at 6.45μm with improved beam quality were demonstrated. Pulsed lasers emitting at around 1μm, e.g. Yb-doped host materials, are frequently employed as pump sources of nonlinear optical conversion schemes. To allow further development of ultrashort pulsed Yb-doped double tungstate lasers, the nonlinear refractive index of several materials was measured. Among these are new materials which were for the first time characterized with regard to their nonlinear refractive index. In addition to the pulsed experiments above, a periodically poled lithium niobate crystal was employed to generate continuous-wave output. Even here, a volume Bragg grating was implemented and thereby demonstrated a novel method to control the threshold of the OPO. Thus, a stable high-energy highly-efficient OPO could be demonstrated.<br><p>QC 20141203</p>

In der vorliegenden Doktorarbeit wird ein Dauerstrich Optisch Parametrischer Oszillator (cw OPO) vorgestellt, der speziell für die hochauflösende Dopplerfreie Molekülspektroskopie und Metrologie entwickelt wurde. Der kontrollierte Zugang zu jeder beliebigen Wellenlänge im breiten Emissionsspektrum von OPOs wie auch das präzise Abstimmen seiner Ausgangsfrequenz über zu untersuchende molekulare und atomare Übergänge stellten lange Zeit Probleme dar, deren Lösung die Grundzielsetzung dieser Arbeit war. Das im Laufe dieser Arbeit entwickelte System hat diese Ziele vollständig erreicht, was durch verschiedene Messungen und Anwendungen demonstriert wurde. Zu diesem Zweck wurde ein neues OPO-Design mit einem Intracavity-Etalon entwickelt und aufgebaut, wobei der OPO auf dem Konzept eines einfach-resonanten cw OPOs mit resonanter Pumpwelle basiert. Die OPO-Ausgangsstrahlung zeigt sehr gute Langzeitstabilität und Spektraleigenschaften, welche durch direkte Frequenzvergleichsmessungen mit einem optischen Methan-Frequenzstandard im Infraroten bestimmt wurden. Eine Idler-Linienbreite von 12 kHz und ein Modensprung-freier Betrieb des OPOs über einen Zeitraum von einigen Tagen wurde beobachtet. Außerdem wurde gezeigt, dass ein OPO zu einer hochstabilen optischen Referenz phasengelockt und somit seine Frequenz sehr genau kontrolliert und durchgestimmt werden kann. Als erste erfolgreiche Anwendung eines OPOs in der Dopplerfreien Spektroskopie wurde ein Aufbau zur Frequenz-Modulationsspektroskopie in Methan realisiert. Weiterhin, wurde der entwickelte cw OPO mit einem femtosekunden optischen Frequenzkamm kombiniert, um eine neue Idee für eine kohärente Verbindung zwischen dem sichtbaren und dem infraroten Spektralbereich zu realisieren. Als erste Demonstration dieser Technologie wurde ein direkter absoluter Frequenzvergleich zwischen einem Jod-stabilisierten Laser bei 532 nm und einem Methan-stabilisierten Laser bei 3390 nm durchgeführt.<br>This thesis presents a continuous-wave optical parametric oscillator (cw OPO), specially developed for high-resolution Doppler-free molecular spectroscopy and metrology. The basic objective was to solve the long-standing problem of controlled access to any desired wavelength in the wide emission range of OPOs, including the ability to precisely tune the output frequency over the molecular and atomic transitions of interest. The system implemented during this work fully achieves these goals and its performance was demonstrated in various measurements and applications. For this aim, a new design for the OPO cavity with an intracavity etalon was implemented, extending the concept of a cw singly resonant OPO with resonated pump wave. The newly developed device demonstrates very good long-term stability and spectral properties, which were determined in direct beat frequency measurements with a methane infrared optical frequency standard. Thus, an idler radiation linewidth of 12 kHz and mode-hop-free operation of the OPO over several days were observed. Furthermore, it was shown that an OPO can be phase locked to a highly stable optical reference and thus much more precisely controlled and tuned. As the first successful application of OPOs in Doppler-free spectroscopy, a frequency modulation spectroscopy setup for detection of sub-Doppler resonances in methane was implemented. Furthermore, the developed cw OPO was integrated with a femtosecond optical frequency comb to realize a new concept for a coherent link between the visible and infrared spectral ranges. As a first demonstration of this technique, a direct absolute frequency comparison between an iodine stabilized laser at 532 nm and a methane stabilized laser at 3390 nm was performed.

Optical parametric oscillators have been known and used for a long time as efficient sources of non-classical states of light both below threshold of oscillation, where they generate squeezed vacuum states and bi-partite entangled states, and above threshold of oscillation, where they generate intensity correlated twin beams. The singly-resonant cavity, where only one of the three field involved in the parametric amplification process is resonated (signal), is in principle a simpler configuration to realize experimentally but, to the best of our knowledge, theoretical investigations of non-classical features of the light from a singly-resonant OPO (SROPO) are missing. One of the reasons is that SROPOs operate with strongly non-degenerate frequencies while much of the literature on squeezing focuses on the degenerate or close to degeneracy cases. Recent interest in non-classical correlations of the strongly non-degenerate regime of parametric down-conversion makes the study of entanglement in SROPO important for the optimization of coherent sources with fluctuations below the shot-noise level. There are clear technical advantages for SROPO configurations: only resonance of the signal field has to be maintained, continuous temperature tuning and suppression of mode-hopping. As a matter of fact even if the doubly resonant configuration, where both the signal and the idler fields are resonated, has a much lower threshold pump power, the tuning behavior is complicated and is massively affected by changes of the crystal temperature or pump wavelength, causing the signal and idler wavelengths undergoing jumps, and the tuning is generally non-monotonous. This is because the operation wavelengths are determined primarily by the requirement for simultaneous resonance for signal and idler, and not only by a phase-matching condition as in the case of singly resonant configuration. It is in this spirit that in Chapter 4 we apply the input-output theory of optical cavities to formulate a quantum treatment of a continuous wave singly-resonant optical parametric oscillator. This case is mainly relevant to largely non-degenerate signal and idler modes. We show that both intensity and quadrature squeezing are present and that the maximum noise reduction below the standard quantum limit is the same at the signal and idler frequencies in a way similar to the doubly resonant case. As the threshold of oscillation is approached, however, the intensity-difference and quadrature spectra display a progressive line-narrowing which is absent in the balanced doubly-resonant case. By using the separability criterion for continuous variables, the signal-idler state is found to be entangled over wide ranges of the parameters. We show that attainable levels of squeezing and entanglement make singly-resonant configurations ideal candidates for two-colour quantum information processes because of their ease of tuning in experimental realizations. Another very interesting feature of SROPOs which, this time, has no counterpart in the doubly-resonant regime is described in Chapter 5 where model equations for the evolution of signal and idler pulses in a synchronously pumped optical parametric oscillator are derived and numerically integrated. A novel regime of giant sub-threshold pulses driven by quantum fluctuations is described through the analysis of stability eigenvalues, growth factors and pseudospectra. Subthreshold pulses driven by quantum fluctuations are found at various mirror reflectivities in the non degenerate regime where signal and idler have different group velocities. Giant sub-threshold pulses open the possibility of observing macroscopic continuous variable entanglement with nonclassical features. This important feature is peculiar to the singly-resonant configuration and has no counterpart in the doubly-resonant regime. Very interesting classical features of SROPOs light are investigated in Chapter 6 where we show that spatio-temporal dynamics of singly resonant optical parametric oscillators with external seeding displays hexagonal, roll and honeycomb patterns, optical turbulence, rogue waves and cavity solitons. We derive appropriate mean-field equations with a sinc² non-linearity and demonstrate that off-resonance seeding is necessary and responsible for the formation of complex spatial structures via self-organization. We compare this model with those derived close to the threshold of signal generation and find that back-conversion of signal and idler photons is responsible for multiple regions of spatio-temporal self-organization when increasing the power of the pump field.

A source-demand in the near- and mid-IR wavelength spectrum exists for various applications such as waveguide inscription, multiphoton imaging, and nonlinear spectroscopy. All of the applications seek for higher repetitions rates for faster processing speed, better signal to noise ratios or to improve the results for applications like laser waveguide inscription. This is in contrast to the high pulse energies, required to drive the nonlinear processes involved with these applications. Available systems are either based on low-energy, high-repetition-rate optical parametric oscillators or high-energy, low-repetition-rate optical parametric amplifiers. In this thesis a sources was developed that can bridge the wide gap between these two extremes, providing sufficient energy to drive nonlinear processes, with repetition rates in the MHz domain. This was achieved by introducing three techniques previously employed for energy scaling in laser cavities. Firstly an exchange from the conventionally used Ti:sapphire pump to a commercial high power Yb:fibre laser system readily scaled the usable pump energy. This was combined with a technique known as cavity-length extension, which allows a lowering of the cavity roundtrip time offering the build-up of pulses with increased energy. In a final stage, cavity-dumping on basis of an acousto-optic modulator was introduced into the a redesigned cavity. The combination of these three techniques, novel to synchronously pumped optical parametric oscillators, enabled the extraction of record-high pulse energies and peak powers

The development of all-solid-state, diode-laser pumped neodymium (Nd) lasers and optical parametric oscillators (OPOs) is described, which realise practical sources of coherent radiation with a high degree of frequency agility, are efficient, reliable and potentially compact. A comparison of various neodymium doped host materials reveals yttrium lithium fluoride (YLF) to be an appropriate replacement for the more widely known host yttrium aluminium garnet (YAG) in diode-laser pumped devices. The development of an end-pumped Nd:YLF laser that utilises a 12-mJ, 60W, quasi-CW diode-laser bar is initially described. Multilongitudinal-mode, TEM00 pulse energies of greater than 2 mJ have been observed, with corresponding peak output powers in excess of 118 kW. The incorporation of a novel pre-lase Q-switching technique has realised single-longitudinal-mode peak powers in excess of 90 kW continuing to be achieved. Further, the development of a more powerful end- pumped Nd:YLF laser utilising 2, 3-bar diode-laser arrays, each providing 72-mJ of pump energy is described. In this case, Q-switched, multilongitudinal-mode, TEM00 pulse energies of greater than 11 mJ are reported, with the clear potential for increasing this to greater than 20 mJ, based on measured fixed-Q pulse energies of greater than 30 mJ. Complementing the development of these diode-laser pumped solid-state lasers is the development of optical parametric oscillators based on the nonlinear materials lithium triborate (LBO) and beta-barium borate (?-BBO). Pumped by the frequency up-converted (third harmonic) output of the mid laser, such optical parametric oscillators introduce extensive frequency agility spanning a spectral range from the deep blue (0.4 mum) to the mid-infrared (2.5 mum). Initially, the development of an LBO based device is reported, which in a type I critical phase- match (CPM) geometry has a measured oscillation threshold of < 0.3 mJ, when pumped by the frequency tripled output of the 144-mJ diode-laser pumped Nd:YLF laser at 0.349 mum. Observed pump depletions are as high as 35%. A similar CPM geometry is reported in beta-BBO, in this case pumped by the frequency tripled and amplified output of a diode-laser pumped Nd:YAG laser at 0.355 mum. This is a more energetic device with thresholds of >5 mJ, but through the introduction of interferometric, dispersive and injection seeding techniques made to operate on a single axial mode. Near transform limited linewidths are reported in devices which continue to have modest pump thresholds and broad tunability. The parametric generation of broad spectral bandwidths (polychromatic) by the use of suitable phase-matching geometries is also reported. Greater than 100 nm simultaneous bandwidth in the visible spectrum is generated in a collimated signal-wave from a novel, noncollinear phase-matching geometry in a beta-BBO optical parametric oscillator, which is pumped by the collimated output of frequency tripled diode-laser pumped Nd:YAG laser. The device is demonstrated to be efficient, having a similar pump threshold and efficiency to that of the well known collinear phase-matched tunable device, and to continue to encompass a degree of tunability allowing the large simultaneous bandwidth to be tuned across the entire visible spectrum. Dispersive cavity tuning of the optical parametric oscillator by the use of a Littrow-mounted grating or acousto-optic tuning filter, with a static crystal and pump configuration, is also described.

This thesis describes research on near degenerate quasi phase-matched opticalparametric oscillators (OPO) where volume Bragg gratings (VBG) are used toproduce narrow oscillation bandwidth. These OPOs are then used to pump a secondOPO to generate mid-infrared radiation. The atmospheric transmission windows in the 3.5 to 5 μm wavelength region areused for seekers on infrared homing missiles. These missiles are available to guerrillaand terrorist groups and have been used in a number of attacks on military and civilianaircraft. Laser sources at the same wavelengths are an important component incountermeasure systems for aircraft self-protection. Similar laser sources also haveapplications in laser surgery. At wavelengths longer than 4 μm crystal materials for multi-Watt level averagepower nonlinear devices is a problem. The best solution so far is to use ZnGeP2(ZGP). ZGP and the available alternatives all have a problem of near-infraredabsorption, and a mid-infrared OPO thus has to use a pump wavelength near 2 μm.This pump source can be a neodymium laser at 1.06 μm with a near degenerate OPO. Nonlinear devices for low to medium pulse energies are dominated by quasi phasematchedmaterials because of their higher effective nonlinearities and lack of walkoff.In addition they allow type I interaction where signal and idler from the OPOhave the same polarization, which has the advantage that both waves can be used topump the ZGP OPO. The drawback of this is that the near-degenerate interaction hasvery wide gain bandwidth. Efficient pumping of the second OPO demands narrowbandwidth output from the first OPO.Volume Bragg gratings that are glass materials with a periodic refractive indexmodulation have emerged as high quality narrow bandwidth reflectors. By using aVBG as one cavity mirror in an OPO the feedback bandwidth and hence the OPOoscillation bandwidth can be kept very narrow. Signal and idler bandwidths of 10 and20 GHz (FWHM) at 2122 and 2135 nm, respectively, have been demonstrated. Thisshould be compared to the several hundred nanometre bandwidth from an OPO usingdielectric mirrors. Very narrow bandwidth operation has been achieved so close todegeneracy that the signal and idler are not resolvable. The total output energy generated in the PPKTP OPO (signal and idler together)has been used to pump a ZGP OPO that produced mid-IR radiation. Tuning of thesignal from a ZGP OPO from 2.9 μm to degeneracy at 4.3 μm has been shown, with acorresponding idler wavelength tuneable up to 8 μm. The highest conversionefficiency that has been reached from 1.06 μm to the mid-IR was 12 %. This setupused a PPKTP OPO with 30 % conversion efficiency and 13 nm separation of signaland idler (2122 and 2135 nm). The pulse repetition frequency was 20 kHz and thegenerated output power in the mid-IR was 3.2 W.<br>QC 20100517

The work described herein concerns the characterisation and development of optical parametric oscillators (OPOs) tunable in the ultraviolet, visible and near infrared regions. These devices were pumped by the 308nm output from line-narrowed Xenon Chloride excimer lasers of pulse energy up to 150mJ. The behaviour of Type 2 phase-matched Urea, and Type 1 phase-matched Barium Borate OPOs in terms of oscillation threshold and conversion efficiency, has been explored. The detrimental effects of pump beam walkoff on the threshold of the critically phase-matched Barium Borate OPO have been quantified. It was found that minimum 17ns pulse energies of 5mJ were required to reach threshold in a device based on a crystal of 20mm length. By contrast, noncritically phase-matched Urea OPOs using crystal lengths of 25mm were operated with as little as 0.6mJ pump energy. A deterioration in performance was observed in both cases with decreasing pump beam waist. Maximum pump depletions of 72% and 64% were observed in Urea and BBO respectively. The useful output from the urea device reached 65%, while higher absorption/scattering losses meant that the useful fraction in BBO was very much lower. Two different types of noncollinear phase-matching were studied in the BBO-OPO. The first recorded observation of operation of a Type 1 OPO at crystal angles beyond the degenerate wavelength point was made. The output took the form of two concentric rings and was attributed to simultaneous singly and doubly resonant operation. Finally, single longitudinal mode operation of the BBO-OPO was demonstrated using a dispersive cavity arrangement. The widely varying inherent linewidth of the device required that different strategies be adopted over different wavelength ranges. Encouraging performance in terms of threshold was observed using the dispersive cavity, and the feasibility of using this device as a low-power first stage for an oscillator/amplifier set-up was studied.

This thesis gives a description of studies relating to the development of continuous-wave (cw) optical parametric oscillators (OPOs) and their application to schemes that require high-precision, narrow-linewidth, and frequency-tunable radiation. There are three separate aims to the work presented within this thesis. First, the requirements on pump sources, nonlinear materials, OPO cavity resonances and phase-matching geometries are analysed with a view to operating cw OPOs with stability above threshold. Second, the results of four distinct experiments are outlined, compared to theory, and discussed within the general context of cw OPO development. Third, this thesis is the first comprehensive review of the above-mentioned performance characteristics of cw OPOs, and focuses on their role as optical frequency dividers within frequency synthesis chains spanning the optical spectrum. The modelling sections highlight the importance of cavity resonances in cw OPOs when evaluating pump power thresholds, conversion efficiencies, and mode-selection properties. Simultaneous signal and idler cavity resonances are shown to be critical when relying upon cw laser sources to reach OPO threshold powers. Such arrangements require the use of stable pump lasers and servo-locked OPO cavity lengths to maintain this doubleresonance condition. There is an in-depth analysis of OPO cavity geometries that can generate frequency-stable and continuously-tunable outputs. The selection of nonlinear materials for cw OPOs is also considered with regard to providing signal and idler frequencies in integral-related frequency ratios, thereby satisfying an important requirement within optical frequency division techniques. Four specific experiments were designed to address many of the issues raised within the modelling sections. These experiments realized the following novel arrangements; the use of lithium triborate as a gain material within cw OPOs; a cw OPO which used a pump source operating in the ultraviolet spectral region; the highest frequency output from a cw OPO; a cw OPO which used a tunable pump source operating in the near infra-red spectral region; multiple parameter pump / OPO coarse frequency tuning; a non- degenerate type II cw OPO phase-matching geometry; and a dual-cavity doubly-resonant cw OPO. Other notable features of the experimental designs included stabilized single-frequency output from a single-cavity cw OPO geometry, continuous frequency tuning from a dual-cavity, doubly-resonant OPO resonator, and the general characteristics of low pump power thresholds and moderate conversion efficiencies. An important feature discussed in detail throughout the thesis is the comparison between type I and type II phase-matching geometries. These two cases give rise to different polarization states for the signal and idler fields within OPO cavities. Type II phase-matching geometries are shown, both in theory and experiments, to be preferable to equivalent type I geometries, when considering stable OPO operation, fine frequency tuning, and multiple cavity oscillators. This is so because type II phase-matching geometries, in general, provide significantly different signal and idler refractive indices which in turn yield a considerable mis-match in the signal and idler free spectral ranges. Subsequently this relaxes the stability requirements within single-cavity doubly-resonant OPOs, and allows for polarization separation to form dual-cavity resonators which are vital to the effective operation of cw OPOs within metrology and spectroscopy. The work contained in this thesis forms an integral part of current research in cw OPOs, a field presently enjoying its most productive and prosperous period. The potential incorporation of cw OPOs within frequency synthesis chains is shown to be dependent on the further development of pump lasers and nonlinear materials. In the short term, the actual use of cw OPOs is assessed in relation to more convenient and widespread techniques for converting, comparing, and measuring absolute frequencies.

Fiber optical parametric amplifiers (OPAs) are based on a highly-efficient four-wave mixing process. Their capability to give very high gain and large bandwidths have made them an attractive candidate for providing higher bandwidths for future telecommunication systems, such as wavelength-division multiplexed (WDM) photonics networks. In dynamic photonic networks a where number of channels are dropped and/or added all the time, the OPA gain for the other channels is affected. In this thesis we employed a well-known gain control technique, all-optical gain clamping (AOGC), and reduced the gain variation of fiber OPAs below 0.5 dB, under varying input conditions. We also showed an improvement in power penalties o at the bit-error rate of 10-8, from 2.5 dB to 0.5 dB for on/off keying modulation. We also investigated fiber optical parametric oscillators (OPOs). Using fiber OPAs as gain medium we realized two different continuous-wave (CW) OPOs, centred at 1561 nm and 1593 nm. One gave us watt-level output power from 1600 nm to 1670 nm, with overall tuning range of 211 nm. The output linewidth of signal and idler was measured to be 0.08 nm and 0.15 nm respectively. The OPO centred at 1593 nm gave us a record tuning range of 254 nm, and with 3 dB output coupling fraction, it gave us large output powers (20-27 dBm) from 1610 nm to 1720 nm. Using a large seed generated by a watt-level fiber OPO in the U-band, and using 3 W of CW pump source in the C-band for Raman amplification, we generated 3 W of CW output power. This gave us nearly 100% conversion efficiency. Launching a high-power CW pump with narrow linewidth into a fiber makes stimulated Brillouin scattering (SBS) a major problem. We investigated an SBS suppressor, based on a common technique of phase dithering of the pump to suppress the SBS. We compared a multitone modulation technique to modulation with a pseudo-random bit sequence (PRBS), and we showed that it can increase the SBS threshold by 4.18 dB, and is less expensive to implement.

Optical source generation has attracted significant attention recently, especially in fiber optical communications. Today there is a growing a demand for optical source generation beyond conventional telecommunication wavelength bands. However, high quality and versatile optical source is generally not available over those wavelength bands due to the lack of efficient gain medium. Thanks to fiber optical parametric amplifier (FOPA), which is based on the third order nonlinear susceptibility of optical fibers, offers ultrafast response, wide-gain bandwidth, high gain and large frequency detune from the pump, serves as a promising candidate for signal amplification over those wavelength bands. By using the corresponding fiber optical parametric oscillator (FOPO) configuration, widely tunable source from continuous-wave (CW) to sub-picosecond pulses can be potentially generated to serve different applications from communication to biomedical imaging. In this thesis, we first demonstrate an all-fiber widely-tunable picosecond FOPO using highly-nonlinear fiber (HNLF). The tuning range is as wide as 250 nm, which is higher than previous picosecond FOPOs reported in the 1550-nm region. Second, time-dispersion tuning of the FOPO is investigated with fixed pump wavelength. It is a relatively simple and economic approach, and there will be no filter induced cavity loss. We then describe using FOPO to generated nearly-transform limited sub-picosecond pulses with a 60-nm tuning range. Another FOPO with a tuning range of 440-nm with dispersion-shifted fiber (DSF) as the gain medium is proposed and demonstrated. Compared with FOPOs demonstrated using HNLF as the gain medium, the use of DSF offers two key advantages: a wider tuning range and a narrower linewidth. In addition to picosecond FOPO, CW FOPO is also of great interest in fiber optical communications and biomedical imaging. We also demonstrate an all-fiber CW single-longitudinal-mode (SLM) FOPO with tuning range covers the S and L bands. SLM oscillation with a side-mode suppression ratio greater than 43 dB is achieved, which has been extended to 1-μm region under stable operation. Apart from static tuning, dynamic wavelength tuning of the FOPO is also discussed in this thesis with a cumulative speed exceeds 4,000,000 nm/s, which is higher than previous work reported in wavelength-swept FOPOs. The high-speed swept source would be useful in biomedical imaging and sensing applications. The amplification of the sub-picosecond pulses of the FOPO output is also investigated, for the first time to our knowledge, by using a fiber optical parametric chirped pulse amplifier(FOPCPA).The totally fiber-integrated nature of the whole system allows complete self-alignment and further integration to other fiber-based systems. All these research effort will show the versatility of FOPO techniques for generating wide range of optical sources for varies applications. These schemes may be useful in generating CW and short pulse for potential optical communication and biomedical imaging in non-conventional wavelength bands.<br>published_or_final_version<br>Electrical and Electronic Engineering<br>Doctoral<br>Doctor of Philosophy

This thesis describes the design, configuration and operation of picosecond optical parametric oscillators (OPOs) tunable from the visible to mid infrared. These systems were based on the materials LiB3O5 (LBO) and KTiOAsO4 (KTA), and were pumped by a self-mode-locked Ti:sapphire laser at a repetition rate of 81 MHz. The initial design of the picosecond parametric oscillator was based on a 16 mm long crystal of LBO. This system produces transform-limited signal pulses with durations of -720 fs. Total average output powers of up to 90 mW over a signal (idler) tuning range of 1.374-1.530 mum (1.676-1.828 mum) have been generated at 1.3 times the 900 mW threshold. The system performance was improved by the use of a new LBO crystal of length 30 mm. This system was continuously tunable from 1.160 to 2.185 mum. Up to 690 mW of output power has been generated for 2 W of input pump power at 5 times threshold. For this output power a depletion of 52 % was achieved with a corresponding external extraction efficiency of 34.5 %. Picosecond pulse generation in the visible by external single-pass frequency- doubling of the LBO OPO to provide picosecond pulses in the 584-771 nm range has been demonstrated. Conversion efficiencies as high as 18 % have been demonstrated, with output powers in excess of 65 mW being measured, when utilising a combination of type I and type II temperature-tuned non-critical phase-matching in LBO. The pulse width of the second harmonic was in the region of 840-880 fs. A further new source of tunable high-repetition-rate picosecond pulses for the visible has also been demonstrated, which is based on an internally-doubled, Ti:sapphire-pumped OPO that uses temperature-tuned LBO both as the OPO and SHG crystal. Oscillation has been obtained for an input pump power of 700 mW with output powers in excess of 320 mW being generated, representing conversion efficiencies of as much as 16 %. The system is continuously tunable from 584 to 771 nm and can provide transform-limited visible pulses with durations of 840-880 fs across the available range. The ability to tune beyond wavelengths of 2.5 mum was also required. To this end a new source of tunable picosecond pulses for the near - to mid - infrared has been developed which is based on the material KTA. Oscillation has been obtained for input pump powers as low as 230 mW. The system produces total output powers in excess of 403 mW with conversion efficiencies of 31 % at 5.2 times threshold. Transform-limited signal (idler) pulses of 1.02 (2.9) ps have been generated over the tuning range 1.139-1.281 (2.377-3.160) mum.

The work presented in this thesis describes the design, configuration and operation of femtosecond optical parametric oscillators based on the materials KTiOPO4 (KTP) and RbTiOAsO4 (RTA) and pumped by a self- modelocked Ti:sapphire laser. The alignment of the pump laser is detailed and thermal effects in the Ti:sapphire rod are examined in the context of a general technique which optimises modelocked performance at any pump power. A KTP-based femtosecond parametric oscillator is described which produces 400-fs-duration signal pulses at an average output power of 150 mW when operated in the absence of group-velocity dispersion- compensation. With intracavity dispersion-compensation, the oscillator produces 40-fs-duration pulses with an average power of 50 mW. Tuning is demonstrated from 1.12 - 1.25 mum in the signal wave and from 2.5 - 3.0 mum in the idler wave by changing only the pump-laser wavelength. Using a novel idler-feedback arrangement, reductions in the oscillation threshold and increases in the signal output power of 10 % are described. Soliton generation in the oscillator is achieved when the net cavity dispersion is positive and results show good agreement with theory. An oscillator using RTA is demonstrated which achieves conversion efficiencies exceeding 30 % and has an operating threshold of only 50 mW. Average signal powers of 100 mW and 185 mW are extracted from the oscillators with and without dispersion-compensation respectively. The corresponding pulse durations are 67 fs and 980 fs and tunability in the signal and idler waves from 1.23 - 1.34 mum and 2.10 - 2.43 mum is demonstrated. Visible output from 620 - 660 nm is obtained by intracavity- doubling and powers of up to 170 mW are measured. These results suggest that RTA has a higher nonlinear coefficient than KTP.

This thesis describes the development of singly-resonant optical parametric oscillators (OPOs) based on the nonlinear material KTP (potassium titanyl phosphate), and used to provide tunable light in the infrared, with low oscillation threshold and high efficiency. Further, the generation of tunable red light by the frequency mixing of the signal wave from the OPO with the pump wave in a non-critical temperature phase-matched lithium triborate crystal (LBO) is reported. We believe this is the first demonstration of such an application of LBO. Two diode-pumped solid-state lasers were used as the pump sources. One was an electro-optically Q-switched Nd:YLF laser which provided high peak power (~600 kW) pulses; and the other one was an acousto-optically Q-switched slab-geometry Nd:YLF laser which provided high repetition rate (1~10 kHz) a.nd low peak power(< 30 kW) pulses. A second version of the acousto-optically Q-switched slab-geometry Nd:YLF laser was designed and constructed with improvements in the pump module and cooling system so as to be much more compact and easier to control. In the first stage of this work, two theoretical models were constructed. One was a model for pump threshold of singly-resonant OPOs for the case of focused Gaussian beams, and was based on Guha's theory. The second one was a model for conversion efficiency of singly-resonant OPOs, for the case of plane waves with pump depletion, and was derived from the coupled wave equations. In the second stage of this work, the effects of beam focusing and Poynting vector walk-off on pump threshold and conversion efficiency for OPOs were extensively studied theoretically and experimentally. Experimental results were found to be in good agreement with theory. The high pump threshold of the critically phase-matched KTP OPO led to several other pump configurations being considered, including intracavity OPOs, cylindrical focusing, and donble-pass of the pump. As a result of the KTP OPO study, very low pump thresholds were achieved in both non-critical phase-matched (NCPM) and critical phase-matched (CPM) KTP OPOs by using long crystal in both intracavity OPOs and the double-pass-pump configuration. Maximum external conversion efficiency from pump to signal was demonstrated to be 37% for the NCPM OPO and 40% for the CPM OPO. The signal wavelength tuning ranges were observed to be 1.54-1.56 mum from the NCPM KTP OPO, and 1.58-1.8 mum from the CPM KTP OPO. In the final stage of this work, the temperature phase-matching properties of LBO were investigated with the use of our measured thermo-optical coefficients of LBO. A particularly interesting result of the investigation is the possibility of sum-frequency generation in non-critically phase-matched LBO with temperature tuning giving considerable wavelength ranges for both the type I and type II geometries. Experimentally, we demonstrated tunalile red light generation by sum-frequency mixing of the 1 mum pump wave and the signal wave of the KTP OPO with an over all conversion efficiency of more than 13%. The wavelength tuning range was observed to 0.62-0.65 mum. The effects of beam focusing on the conversion efficiency for sum-frequency generation were analysed theoretically, and several opportunities for further improvement were shown clearly from this analysis.

I den här avhandlingen visas hur lasrar och optiska parametriska oscillatorer (OPO:er) kan styras spektralt med hjälp av volymbraggitter. Volymbraggitter utgörs av ett periodiskt varierande brytningsindex som skrivits i ett fototermorefraktivt glas. Gittret reflekterar därmed en specifik våglängd som bestäms av perioden hos modulationen, och kan tillverkas med smal bandbredd och hög reflektans beroende på modulationens längd och styrka. En teoretisk modell har utvecklats för reflektiva volymbraggitters egenskaper om den infallande strålen har en större vinkelspridning än gittrets vinkeltolerans. Detta kan bl.a. inträffa i en laserkavitet där gittret används vid snett infall, och en teoretisk beskrivning är därför ett viktigt redskap för att kunna designa sådana lasrar. Spektral kontroll av ett antal fasta tillståndslasrar med hjälp av volymbraggitter har i försök påvisats, och lasern har därvid både kunnat avstämmas spektralt samtidigt som en avsmalnad spektral bandbredd erhållits. Lasern kan göras väldigt enkel genom att byta ut en av kavitetsspeglarna mot gittret. Tack vare gittrets goda spektrala urvalsmekanism kan lasern låsas var som helst i förstärkningsspektrumet. De tekniker och lasrar som demonstrerats experimentellt är följande: Lasring i en enda longitudinell mod erhölls både för en diodpumpad ErYb:glas-laser vid 1553 nm med ca 10 mW:s effekt och 90 kHz linjebredd samt för en diodpumpad Nd:GdVO4-laser vid 1066 nm med 0.85 W:s effekt. Lasrarnas våglängd kunde avstämmas över större delen av gittrets bandbredd på ca. 30 GHz. Genom att bygga Nd:GdVO4-lasern med en monolitisk kavitet kunde även en spektralt synnerligen stabil laser erhållas med under 40 MHz bandbredd. Tillämpningar för dessa lasrar finns både inom spektroskopi samt som källor för intrakavitetsfördubbling till synliga våglängder. Genom att använda gittret som inkopplingsspegel går det även att framställa lasrar med en väldigt låg kvantdefekt, som därför får minskad värmeutveckling i lasermediet. Detta medger i sin tur att lasrar med höga medeleffekter kan konstrueras, som kan användas bl.a. för olika former av materialbearbetning. I detta arbete har lasrar med låg kvantdefekt byggts med Yb:KYW som laserkristall; både en laser vid 998 nm på 3.6 W som diodpumpades vid 982 nm och med en bandbredd på 10 GHz, samt en laser vid 990 nm på 70 mW som pumpades av en Ti:safir-laser vid 980 nm. Om volymbraggittret används vid snett infall kan den reflekterade våglängden avstämmas genom att gittret roteras. Denna princip användes i en diodpumpad Yb:KYW-laser till att erhålla en brett avstämbar laservåglängd mellan 996 nm och 1048 nm med en maximal effekt på 3 W och med 10 GHz bandbredd. Genom att placera gittret i en retroreflektor kunde avstämningen göras utan att kaviteten behövde linjeras om. En laser som denna kan exempelvis användas för olika typer av materialkarakterisering och spektroskopi. Med optiska parametriska oscillatorer (OPO:er) kan laserljus omvandlas till nya våglängder. Därmed kan OPO:er användas som koherenta ljuskällor där inga effektiva lasrar existerar. OPO-processen kan göras effektiv om en pulsad pump används, och den genererade våglängden kan enkelt styras med hjälp av periodiskt polade (PP) icke-linjära kristaller, såsom PP-KTiOPO4, som användes i detta arbete. En nackdel med OPO:er är att i allmänhet är den genererade signalen tämligen spektralt bredbandig. Signalens bandbredd kan dock avsmalnas betydligt om ett spektralt filter såsom ett volymbraggitter används. Genom att byta ut en av speglarna i OPO-kaviteten mot gittret kan utformningen av OPO:n göras väldigt enkel. I en OPO med en signalvåglängd på 975 nm kunde en avsmalning av bandbredden till 50 GHz påvisas med hjälp av ett braggitter. Detta motsvarar 20 gångers minskning jämfört med om en konventionell spegel används. Som mest erhölls en pulsenergi på 0.34 mJ i signalen. Genom att rotera gittret kunde våglängden avstämmas 21 THz. För att förenkla avstämningen konstruerades även en OPO med gittret i en retroreflektor, samtidigt som kaviteten var av ringtyp. I denna OPO vid en våglängd på 760 nm och med en pulsenergi i signalen på upp till 0.42 mJ erhölls en bandbredd på 130 GHz och ett avstämningsområde på 2.6 THz. Slutligen har en OPO vid 1 µm konstruerats med ett gitter med en transversellt varierande period, s.k. chirp. Därigenom kan våglängden avstämmas väldigt enkelt genom att bara flytta gittret transversellt. En tillämpning av dessa OPO:er är såsom ljuskällor i olika typer av laserbaserade sensorer, i vilka en specifik och stabil våglängd erfordras. Dessutom kan de smalbandiga OPO:erna användas som första steg i ickelinjära processer i flera steg. Smal bandbredd är då viktig för effektiviteten i den påföljande ickelinjära omvandlingen i nästa steg.<br>The object of this thesis is to explore the usage of reflective volume Bragg gratings in photo-thermo-refractive glass for spectral control of solid-state lasers and optical parametric oscillators, to build tunable and narrowband coherent light-sources. In order to provide a design tool for use of reflective volume Bragg gratings in laser cavities, a theory was developed that describes the performance of the gratings if the incident beam has finite width with an angular spectrum that is comparable to the grating's angular acceptance bandwidth. Spectral control was demonstrated in a number of cw solid-state lasers, in terms of narrow bandwidth and tunable wavelength, by use of a volume Bragg grating. The design could be made very simple by replacing one of the cavity mirrors with the grating. Thanks to the grating's strong spectral selectivity, the lasers could be locked anywhere in the gain spectrum, while the laser bandwidth was substantially narrowed. In particular, the following lasers were demonstrated: Single-longitudinal-mode lasing in ErYb:glass at 1553 nm with 90 kHz linewidth and in Nd:GdVO4 at 1066 nm with a linewidth below 40 MHz. Very low quantum defect in Yb:KYW lasers, diode-pumped at 982 nm and lasing at 998 nm with 10 GHz bandwidth, as well as Ti:sapphire-pumped at 980 nm and lasing at 990 nm. An Yb:KYW laser that was widely tunable from 996 nm to 1048 nm with 10 GHz bandwidth. In nanosecond pulsed optical parametric oscillators (OPOs) based on periodically poled KTiOPO4, narrowband operation and a tunable wavelength were demonstrated with a volume Bragg grating as a cavity mirror. At a signal wavelength of 975 nm, the bandwidth was 50 GHz, a reduction by 20 times compared to using a conventional mirror. A tuning range of 21 THz was also demonstrated. In another OPO at a signal wavelength of 760 nm, a ring-cavity design was demonstrated to provide convenient tuning. A tuning range of 2.6 THz and a bandwidth of 130 GHz was shown. Also, narrowband operation and tuning in an OPO around 1 µm was demonstrated by use of a transversely chirped Bragg grating.<br>QC 20100813

This thesis describes the development and applications of single-frequency, continuously tunable, continuous-wave (cw), optical parametric oscillators (OPOs). Two doubly-resonant OPOs (DROs) are presented, one providing tunable light around 1?m, the other specifically designed as a spectroscopic source for methane near 1649nm. Once stabilised, the frequency-selective nature of the DRO ensures operation on a single mode-pair without the need for additional intracavity frequency-selective components. Both DROs are smoothly tunable by smoothly tuning the pump laser. The 1mum DRO is based on a bulk KTP crystal cut for near-degenerate, type-II, critical phase-matching (theta= 90&deg;, &phiv; = 37&deg;). Angle tuning the crystal provides coarse tuning of the output frequencies over a range of ~50nm. Small perturbations to the OPO cavity is sufficient to cause a systematic mode-hop and provides a method of tuning across the phase-matching bandwidth (~0.5THz). This DRO is demonstrated as a spectroscopic source by recording the absorption spectrum of cesium molecules near 1050nm. The DRO as a potentially compact source of tunable light is demonstrated by using a frequency-doubled microchip laser as the pump source. The output consists of a single pair of signal and idler modes even when using a multilongitudinal-mode pump laser. Smooth tuning of the output frequencies is achieved by temperature tuning the pump laser. The 1.65mum DRO is based on periodically poled KTiOPO4 (PPKTP). The suitability of PPKTP for cw OPOs was first assessed by a difference frequency generation experiment from which the effective d33 coefficient was estimated to be ~5mum/V. The idler wavelength is coarsely tuned at a rate of 0.73nm/&deg;C by varying the crystal temperature. A combination of computer modelling and experimental observation is used to study the dynamic behaviour of a DRO. The numerical model calculates the time required for the OPO to build-up from the parametric fluorescence and is in excellent agreement with experimental observations.

This thesis presents the development of a new class of high-power, continuous-wave (cw) optical parametric oscillators (OPOs) with extended tunability from visible to near-infrared (near-IR). While lasers have been in use for nearly 50 years, it is still difficult to develop laser systems that can cover many regions of the optical spectrum, from ultraviolet (UV) and visible to the near and mid-infrared wavelength range, with potential applications in the fields such as spectroscopy, remote sensing, trace gas detection, and many more. Development of cw OPOs in singly-resonant oscillator (SRO) configurations, the focus of this thesis, is challenging due to the high threshold pump power (several watts). In addition, with visible pumping, photorefractive effect and thermal lensing effects become important issues to overcome. Therefore, the realization of practical cw SROs requires optimal cavity design, suitable nonlinear materials, and high-power laser with high spectral and spatial quality. High-power, single-frequency, cw SROs based on 30-mm-long MgO-doped, stoichiometrically grown, periodically-poled LiTaO3 (MgO:sPPLT) have been developed. The oscillators were pumped in the green by a frequency-doubled cw diode-pumped Nd:YVO4 laser at 532 nm. With a single grating period of 7.97 µm, continuous signal and idler coverage over 848-1430 nm is obtained by temperature tuning between 52 oC and 248 oC. In a linear cavity configuration and double-pass pumping, an oscillation threshold of 2.88 W has been obtained, and single-pass idler powers in excess of 1.51 W have been generated over 1104-1430 nm for 6 W of pump power at an extraction efficiency of 25.2% and photon conversion efficiency of 56.7%. For single-frequency performance of the cw SRO across 848-1430 nm, we have used a compact ring cavity configuration along with a frequency selecting element (etalon). Using the same MgO:sPPLT crystal, the SRO oscillation threshold of 2.84 W has been obtained, and single-pass idler powers in excess of 1.59 W have been generated over 1104-1430 nm with a maximum SRO extraction efficiency of 25.2% and pump depletions as much as 67%. The single-frequency idler output has a linewidth of ~7 MHz. Under free-running conditions and in the absence of thermal isolation, the idler power exhibits a peak-to-peak stability of 16% over 5 hours. Although the cw SRO can provide optical radiation across 848-1430 nm, the high output power was only available over 1104-1430 nm, due to the high reflectivity of the cavity mirrors for SRO operation. Using finite output coupling of the resonant wave, we have extended the available practical output power across the entire tuning range. The cw out-coupled SRO (OC-SRO) can deliver total power of up to 3.6 W at 40% extraction efficiency with a linewidth of 3 MHz across 848-1430 nm. The signal power shows a peak-to-peak power stability <10.7% over 40 minutes in a TEM00 spatial mode with M2 <1.52. Without any active stabilization, the resonant signal exhibits a natural long-term frequency stability <75 MHz over 15 minutes and short-term frequency stability <10 MHz over 10 seconds, demonstrating the potential of the system for spectroscopic applications. Using internal second-harmonic-generation of the resonant near-infrared signal radiation of the MgO:sPPLT cw SRO in a 5-mm-long BiB3O6 crystal, we have generated 1.27 W of cw, single-frequency blue power over a tunable range of 425-489 nm with a linewidth of 8.5 MHz and a Gaussian spatial beam profile. The blue source is frequency-stable to better than 280 MHz, limited by the resolution of the wavemeter. We have also developed cw green sources, in a simple single-pass experimental configuration by frequency-doubling a fiber laser using MgO:sPPLT and periodically-poled KTiOPO4 (PPKTP) crystals, generating as much as 9.6 W of green radiation in TEM00 spatial beam profile (M2 <1.33) with a single-pass efficiency of 32.7% in MgO:sPPLT. This green source has also successfully been used to pump cw SROs and will be used to pump Ti:sapphire lasers. Using this frequency-doubled green source, we have demonstrated cw OC-SRO providing a stable single-frequency output power up to 2 W across the tuning range of 855-1408 nm, with peak-to-peak power stability <11.7%, frequency-stability <10 MHz over 10 seconds, in TEM00 (M2 <1.26) spatial beam profile.<br>Esta tesis presenta el desarrollo de una nueva clase de osciladores ópticos paramétricos (OPOs) de onda continua (cw) y alta potencia con extendida sintonización desde el visible al infrarrojo (IR) cercano. A pesar de que los láseres están en uso desde hace casi 50 años, todavía es difícil desarrollar sistemas láser que puedan cubrir muchas regiones del espectro óptico en los rangos de longitud de onda desde el ultravioleta (UV) y visible hasta el infrarrojo cercano y medio, con potenciales aplicaciones en campos como la espectroscopia, sensores remotos, detección de trazas de gases, entre muchas otras. El desarrollo de cw OPOs en configuraciones de oscilador simplemente resonante (SRO), objetivo principal de esta tesis, es un gran desafío debido al alto umbral de potencia de bombeo (varios watts). Además, cuando se emplea bombeo visible, los efectos fotorrefractivo y de lente térmica adquieren especial relevancia y son difíciles de superar. Por lo tanto, la realización de cw SROs prácticos requiere de un óptimo diseño de cavidad, adecuados materiales no lineales y láseres de alta potencia con excelente calidad tanto espectral como espacial. Se han desarrollado cw SROs de alta potencia y frecuencia única basados en cristales de LiTaO3 de 30 mm de longitud, de crecido estequiométrico, con dopado de MgO y periódicamente pulidos (MgO:sPPLT). Los osciladores fueron bombeados en el verde mediante el láser de cw Nd:YVO4 bombeado por diodos y doblado en frecuencia. Utilizando un único periodo de red de 7.97 m, se ha obtenido cobertura continua de los campos señal y pivote en el rango 848-1430 nm por sintonización de temperatura entre 52ºC y 248ºC. Empleando una configuración de cavidad lineal y bombeo de doble paso, se ha logrado un umbral de oscilación de 2.88 W y se han generado potencias superiores a 1.51 W para el campo pivote en simple paso dentro del rango 1104-1430 nm para 6 W de potencia de bombeo, eficiencia de extracción del 25.2% y eficiencia de conversión de fotón del 56.7%. Con el objetivo de operar el cw SRO en frecuencia única a través del rango 848-1430 nm, hemos utilizado una configuración compacta de cavidad en anillo junto a un elemento para la selección de frecuencia (etalon). Utilizando el mismo cristal de MgO:sPPLT, se ha obtenido un umbral de oscilación del SRO de 2.84 W y se han generado potencias superiores a 1.59 W para el campo pivote en paso único dentro del rango 1104-1430 nm con una eficiencia máxima de extracción del 25.2 % y agotamiento del bombeo tan alto como el 67%. La salida del campo pivote en frecuencia única tiene un ancho de línea de ~ 7 MHz. Bajo condiciones de sistema libre y en ausencia de aislamiento térmico, la potencia del campo pivote exhibe estabilidad de pico a pico de 16% durante 5 horas. A pesar de que el cw SRO puede proveer radiación óptica en el rango 848-1430 nm, la alta potencia de salida solo se consiguió obtener en el rango 1104-1430 nm a causa de la alta reflectividad de los espejos de la cavidad para operar en SRO. Utilizando un acoplamiento de salida finito de la onda resonante, hemos extendido la disponibilidad de prácticas potencias de salida a través de todo el rango de sintonía. El cw SRO con acoplador de salida (OC-SRO) puede entregar un apotencia total de hasta 3.6 W con una eficiencia de extracción del 40% y con un ancho de línea de 3 MHz en el rango 848-1430 nm. La potencia del campo señal muestra fluctuaciones en potencia de pico a pico <10.7% durante 40 minutos y modo espacial TEM00 con M2<1.52. En ausencia de estabilización activa, el campo señal resonante exhibe una estabilidad en frecuencia natural a largo término con fluctuaciones <75 MHz durante 15 minutos, así como a corto término con fluctuaciones<10MHz durante 10 segundos, demostrando el potencial del sistema para aplicaciones en espectroscopia. Utilizando generación interna de segundo harmónico del campo señal resonante en el rango del infrarrojo cercano del MgO:sPPLT cw SRO mediante un cristal de BiB3O6 de 5 mm de longitud, hemos logrado generar 1.27 W de potencia cw y frecuencia única en el azul dentro del rango de sintonía 425-489 nm y con un ancho de línea de 8.5 MHz y un perfil espacial del haz de tipo Gaussiano. La estabilidad en frecuencia de la fuente azul es mejor que 280 MHz, donde la limitación viene impuesta por la resolución del medidor de longitud de onda empleado. Adicionalmente, hemos desarrollado fuentes verdes en cw en una sencilla configuración experimental de único paso, mediante el doblado en frecuencia de un láser de fibra con cristales de MgO:sPPLT y KTiOPO4 pulido periódicamente (PPKTP), generando hasta 9.6 W de radiación verde en modo espacial TEM00 (M2<1.33) con una eficiencia de paso único de 32.7% en MgO:sPPLT. Esta fuente verde has sido también empleada exitosamente para bombear cw SROs y será utilizada para bombear láseres de Ti:sapphire. Mediante esta fuente verde doblada en frecuencia, hemos demostrado que el cw OC-SRO proporciona una salida estable en frecuencia única con potencia de hasta 2 W a través del rango de sintonía 855-1408 nm, con estabilidad en potencia de pico a pico <11.7%, estabilidad en frecuencia <10 MHZ durante 10 segundos y modo espacial TEM00 (M2<1.26).

The advent of new quasi phase matched materials and high spectral/spatial quality pump sources has led to a renaissance in the development of continuous-wave optical parametric oscillators for the coherent generation of broadly tunable light in the mid infrared spectral region. This thesis describes a novel technique which overcomes the threshold constraints of the singly resonant oscillator (SRO) and stability constraints of the doubly resonant oscillator (DRO) traditionally associated with these devices by placing a singly resonant optical parametric oscillator in the high circulating field found within the cavity of a laser: the intracavity optical parametric oscillator. An SRO based upon the nonlinear material periodically poled LiNb03 (PPLN) operating internal to an all solid state, 1W diode pumped Nd:YV04 mini-laser is demonstrated and characterised. This system exhibits SRO threshold at only 330mW of external diode pump power, and produced a total of 70mW of extractable idler at 1W diode pump power. Through multi-parameter tuning of the poled nonlinear material we demonstrate broad tuning of the non-resonant idler through the spectrally important range 3.1 - 4μm. Novel cavity design desensitises the system to the effects of thermal lensing in the nonlinear medium, resulting in stable spatial and mean power outputs. The short term pump field stability is characterised by intensity modulation brought about by the onset of relaxation oscillations ; a consequence of placing the SRO within the cavity of the pump laser. A comparative study of SRO's based upon PPLN and the new material periodically poled RbTi0As04 (PPRTA) pumped internal to a high power fibre coupled diode pumped Nd:YV04 laser cavity is undertaken and presented. We see that although the nonlinearity and interaction length of the PPRTA is smaller than that of PPLN, the system based upon PPRTA outperforms or is at least comparable with that based upon PPLN in every respect with the exception of idler tuning range. We attribute this to the reduced sensitivity of this material to the effect of thermal lensing. Up to 440mW of extracted idler was produced by each system. The reduction of interferometric feedback of the pump field by the signal cavity mirror was found to eliminate the onset of relaxation oscillations in the case of PPRTA but not PPLN, due to thermal air currents dominating the triggering process in iii this system. Recently published Sellmeier equations and temperature derivatives for PPRTA are compared with the experimentally observed temperature tuning behaviour. The inclusion of an optical parametric oscillator within the cavity of the pump laser impacts significantly upon the transient dynamics of the pump laser in which it resides. We show experimental evidence of this effect and outline a strategy to minimise the effects of relaxation oscillations in the context of a simple numerical model which shall be derived. Possible future avenues of research are discussed in the context of the results and conclusions obtained over the course of this research program.

This thesis reports investigations of several configurations of high pump power, cw-mode-locked synchronously pumped optical parametric oscillator (SPOPO). The focus is on singly resonant, picosecond-domain systems, including: (1) a SPOPO based on periodically poled lithium niobate (PPLN), equipped with a diffraction grating to tune within the gain bandwidth; (2) a PPLN SPOPO designed to operate at long idler wavelengths, where the idler experiences strong attenuation; (3) a SPOPO based on cadmium selenide (CdSe), pumped in tandem by a 1-μm-pumped PPLN SPOPO. The primary pump source used is a Nd:YLF oscillator-amplifier system (λ = 1.047 μm), delivering ~ 4-ps pulses at 120-MHz repetition rate to the SPOPOs. Details of this source, used in conjunction with a standard configuration of PPLN SPOPO, are presented, including modifications to the amplifier stage to extract higher output power. Several aspects of the SPOPO performance related to later work are examined, including generation of extra spectral content, idler characterisation and cavity-length-dependent pulse compression. The diffraction grating provides a means of agile tuning, as well as providing general benefits to SPOPO operation, including suppression of extra spectral content in the signal, suppression of cavity-length dependent effects such as pulse compression and frequency drift, and a significant increase in cavity-length tolerance. Asymmetry of the tuning curves is examined and attributed to non-collinear phase-matching components. The long-idler-wavelength operation of a PPLN SPOPO is then presented, a strategy for this regime being minimisation of signal losses in the cavity. Preliminary results are presented, including tuning out to ~ 7.3 μm, and ~ 0.5 mW of average power measured at 7-μm. Finally, a tandem-pumped, noncritically phase-matched CdSe SPOPO is demonstrated. By varying the pump wavelength, idler tuning was achieved over the range 9.1-9.7 μm and average output powers of up to 40 mW were recorded, with significant scope for wider tuning and power scaling.

Ce manuscrit porte sur la génération de lumière infrarouge paramétrique dans la gamme de longueurs d'onde 1-12 microns, et qui reste à ce jour un défi à l'interface entre les disciplines de l'optique non-linéaire et des sciences des matériaux. Historiquement, c'est la stratégie de l'accord de phase par biréfringence (APB) dans les matériaux anisotropes qui s’est avérée la plus efficace. Mais depuis les années 1990, le succès du quasi-accord de phase (QAP) a permis l’obtention rendements de conversion plus élevés tout en ouvrant de nombreuses possibilités d'accordabilité en longueur d'onde du rayonnement émis, conduisant naturellement à un regain d’intérêt pour les Oscillateurs Paramétriques Optiques (OPO).Nous avons construit le premier OPO nanoseconde en quasi-accord de phase angulaire à base d'un cristal de 5 millimètres d'épaisseur de 5%MgO:PPLN usiné sous la forme d'un cylindre partiel. L'accordabilité angulaire et continue, sans régulation thermique, de cet OPO s'étend de 1.4 jusqu'à 4.4 microns. Dans ce travail, nous avons montré que la configuration des vecteurs d'onde entre l'onde de pompe et les ondes générées dans la cavité était colinéaire et qu’une optimisation de la longueur de cavité permettait d'obtenir des performances énergétiques équivalentes à celles d'un OPO à base d'un cristal traité antireflet et de forme parallélépipédique. Des efficacités de conversion globales supérieures à 30% ont ainsi été obtenues correspondant à une énergie par impulsion supérieure à 2 mJ sur toute la gamme d'accordabilité.Lorsque deux tels OPOs sont pompés de manière synchrone par le même laser de pompe, nous disposons d'une source de Différence de Fréquences (DFG) hautement polyvalente permettant d'envisager des expériences de conversion de fréquences aussi bien en accord de phase par biréfringence qu’en quasi-accord de phase. Les premières expériences de DFG en APB ont été réalisées dans un cristal de Séléniure de Cadmium (CdSe) de 4 cm de long orienté pour l'accord de phase non-critique, et à deux longueurs d'onde de pompe différentes: 2.72 µm et 2.79 µm. Nous avons ensuite conduit des expériences de conversion de fréquences dans un cristal cylindrique de CdSe de 5 mm de diamètre. L'emploi d'une longueur d'onde de pompe de 2.79 microns nous a permis d'accorder la longueur d'onde générée par DFG entre 8.3 et 10.3 µm en tournant le cristal sur une gamme angulaire de 18°. La mise en place de techniques de rétrécissement spectral des OPOs est anticipée et permettra une amélioration de la précision des mesures des longueurs d'onde d'accord de phase ainsi qu'une augmentation significative des rendements de conversion de DFG.Ces expériences de différences de fréquences sont des premiers résultats encourageants et doivent permettre d'accélerer l'identification et la caractérisation de nouveaux matériaux en vue de la construction de sources compactes et accordables sur l'ensemble du spectre infrarouge. C'est en particulier le cas pour CdSiP2 dont les potentialités en termes d'accord de phase non-critique sont importantes lorsqu'il est pompé à 1.064 µm mais qui présente des caractéristiques tout à fait excitantes du point de vue de la génération de supercontinuum lorsqu'il est pompé à 2.4 µm. D'un point de vue plus fondamental, la capacité de réaliser des expériences de DFG à différentes longueurs d'onde de pompe dans l'infrarouge moyen (1- 3 µm) doit permettre de déterminer les indices de réfraction d'un matériau dans l'infrarouge lointain (5 - 50 µm). Nous avons en effet imagine une nouvelle méthode qui utilise les mesures des angles d'accord de phase de DFG d'un cristal pour remonter à la valeur de ses indices principaux dans des gammes spectrales où les mesures directes sont très délicates. Cette nouvelle méthode utilise les mesures inédites de DFG dans des cristaux usinés sous forme de sphère ou de cylindres et devrait permettre de nouvelles avancées dans le domaine de la métrologie de l'accord de phase<br>This dissertation deals with the generation of parametric light in the range 1 to 12 µm. Parametric infrared generation turns out to be a challenge at the interface between the fields of nonlinear optics and materials science embodied by the two approaches used to achieve efficient frequency conversion. Birefringent Phase-Matching (BPM) in anisotropic materials has been the traditional solution used in most frequency converter devices. But since the 90's, the quick success of microstructured materials has paved the way for Quasi-Phase-Matching (QPM) even in isotropic materials, leading to a renewed interest in Optical Parametric Oscillators (OPO). The high degree of engineering offered by this technology is now widely recognized as a key competitive advantage. We obtained original results concerning parametric infrared generation using BPM as well as QPM.We have built the first OPO pumped by a 1.064 µm Nd:YAG laser and based on a 5-mm-thick crystal of 5%MgO:PPLN cut as a partial cylinder. This OPO combines a wide and continuous tunability over the range 1.4 µm - 4.4 µm with a good conversion efficiency, up to 30%. Despite the need to resort to pump intensities almost an order of magnitude higher than in a slab OPO, we have shown that the energetical performance of a partial cylinder OPO is now equivalent to that of a slab OPO besides a wider tunability that can be continuously addressed. When the same Nd:YAG laser pumps two such independent OPOs in parallel, we dispose of a highly versatile QPM dual wavelength source with two widely and independently tunable beams. We have built this unique source allowing versatile Difference Frequency Generation (DFG) towards the mid- and far- infrared. We carried out the first BPM DFG experiments with this source in a CdSe slab oriented for angular noncritical phase-matching at two different pump wavelengths, respectively 2.72 µm and 2.79 µm. The second set of DFG experiments were performed in a CdSe crystal cut and polished as a 5-mm-diameter full cylinder. Using a pump wavelength of 2.79 µm, we were able to tune the DFG wavelength from 8.3 µm up to 10.3 µm by rotating the crystal over an angular range of 18°. Contrary to all the BPM DFG experiments reported so far in the single crystal CdSe, tuning was achieved while keeping normal incidence of both the incident and generated beams in the crystal. The implementation of spectral narrowing techniques is already anticipated and will contribute to more accurate measurements of the phase-matching directions of a crystal as well as to a higher DFG conversion efficiency.These experiments with our dual wavelength source are preliminary and encouraging validations of our capability of performing DFG in small crystals and at any pump wavelength between 1.4 µm and 3.5 µm. Even though we investigated the promises held by CdSiP2 when it is only pumped with a Nd:YAG laser at 1.064 µm, there is tremendous prospect in terms of tunable infrared generation between 3.5 µm and 8 µm when this crystal is pumped around 2.4 µm. Such early demonstrations will be highly valuable for future applications requiring compact and tunable sources spanning the infrared spectrum. From a more fundamental point of view, performing DFG experiments at different pump wavelengths in the mid-infrared can lead to a highly accurate determination of the values of the refractive indices of a nonlinear crystal. In this dissertation, we have cast the first stone of a method that leads to the determination of the values of the refractive indices of a nonlinear crystal in the mid- to far- infrared. This new method is based on the unique measurements of the DFG phase-matching angles in spheres or cylinders, and should contribute to further advances in the field of phase-matching metrology

This thesis is concerned with investigating the generation of ultra short, tunable pulses at high average power and / or high pulse energy using synchronously pumped optical parametric oscillators (OPO) and appropriate power-scalable fibre-amplifier pump sources. Two types of pump sources with average powers up to ≈ 100W are considered: (1) a picosecond, allfiberised, high-power, variable-repetition-rate, Yb:fibre-amplified, gain-switched laser diode system and (2) a femtosecond, high-power, chirped-pulse amplification Yb:fibre laser system incorporating a pulse shaper module. Such OPO systems find applications in fields as diverse as materials processing and nonlinear microscopy / spectroscopy. Two OPOs based on periodically poled lithium niobate (PPLN) and pumped at 1060 nm from the first pump source are demonstrated. With 20 ps-long pump pulses, average powers of up to 7.3W (3.1W) for the signal (idler) are generated at variable repetition rates of ≈ 0.1 . . . 1GHz. With longer 100 ps pump pulses at a repetition rate of < 8MHz and an intracavity fibre as an OPO feedback component for compactness, combined pulse energies approaching 1 μJ are obtained, which are the highest reported to date. Tuning ranges from 1.4 μm to 1.7 μm (signal) and from 2.8 μm to 4.4 μm (idler) are typical for both OPOs. Including frequency-doubling of the 1060 nm light, the first pump source, operating at 230MHz and 20 ps, is used for two green-pumped OPOs tunable in the near-infrared range from 650 nm to 1040 nm(plus the idler from1.08 μmto 2.9 μm). The first OPO uses MgO-doped PPLN and up to 270mW of combined output power with 1W of pump power is obtained. Operation at higher power is complicated due to damage effects such as photo-refraction, nonlinear or induced absorption in lithium niobate. The second OPO uses lithium triborate (LBO) and compressed 4.4 ps green pump pulses to generate record average powers of up to 3.7W of signal and 1.8W of idler. Using the second pump source with a liquid crystal spatial light modulator pulse shaper, the demonstration of energy-scalable output pulses from 0.1 μJ to 2 μJ at a centre wavelength of 1045 nm with typical pulse durations between 300 fs and 600 fs is reported. Pump pulses with a duration of ≈ 600 fs at a repetition rate of 50MHz from this pump source are used for a PPLN OPO producing ≈ 1.9W (≈ 1.2W) of signal (idler) power at 1.5 μm (3.6 μm)

High-power, continuous-wave (cw), mid-infrared (mid-IR) laser sources are of interest for variety of applications such as trace gas detection and remote sensing, which require broad spectral coverage to address the most prominent absorption features of a wide range of molecular species particularly in the mid-IR fingerprint region. On the other hand, surgical applications require high energy sources with unique pulse structure at specific wavelength in the mid-IR ranging from 6-6.5 m. Optical parametric oscillators (OPOs) offer potential sources for all the above applications. The output wavelengths of a singly-resonant oscillator (SRO) can be coarsely tuned over wide ranges through the adjustment of the nonlinear crystal temperature, phase-matching angle or, in the case of quasi-phase-matched (QPM) the first time. The high-energy CSP OPO marked the first demonstration of a compact, high-repetition-rate OPO synchronously pumped by a master oscillator power amplifier system at 1064 nm, generating an milli-joule pulses in the 6-6.5 m spectral range, which is technologically important for surgical applications. Additionally, we also demonstrated a fiber-based-green source at 532 nm, based on single-pass second harmonic generation (SHG) in MgO:sPPLT, as an alternative pump source for Ti:sapphire laser, pointing towards the future, compact fiber-laser pumped Ti:sapphire lasers. Further efforts to improve the SHG efficiency led to the development of a novel multi-crystal scheme, enabling single-pass SHG efficiency as high as 56%. This generic technique is simple and can be implemented at any wavelength. materials, the QPM grating period. The combination of SRO with a tunable pump laser allows the development of uniquely flexible and rapidly tunable class of mid-IR sources. In this thesis we have demonstrated several mid-IR OPOs in the cw as well as ultrafast picosecond regime pumped by fiber-lasers making them compact and robust. In the cw regime, we developed a high-power, Yb-fiber-laser pumped mid-IR OPO based on MgO:PPLN spanning 1506-1945 nm in the near-IR and 2304-3615 nm wavelength range in the mid-IR, efficiently addressing the thermal effects by implementing the optimum signal output coupling. Novel materials such a MgO:sPPLT, with better optical and thermal properties for cw mid-IR generation are explored. High-power broadband, cw mid-IR generation is also demonstrated by using the extended phase-matching properties of MgO:PPLN. Further, we also demonstrated a simple, inexpensive and novel interferometric technique for absolute optimization of output power from a ring optical oscillator. We deployed a picosecond Yb-fiber-laser pumped mid-IR OPO based on MgO:PPLN in ring cavity configuration to demonstrate this proof-of-principle experiment for<br>Fuentes coherentes de luz continua y de alta potencia en el infrarrojo-medio (mid-IR) son de gran interés por su aplicación en la detección de gases, detección remota y la observación de imágenes. Estas aplicaciones requieren un ancho de banda amplio para evidenciar las características que ofrece la absorción de una gran variedad de especies moleculares, particularmente en la región “finger print” del mid-IR. Por otra parte, fuentes altamente energéticas con pulsos que posean estructuras peculiares en rangos específicos de longitud de onda en el mid-IR, entre 6-6.5 m. , prometen características únicas para nuevas aplicaciones en cirugía. Osciladores ópticos paramétricos (OPOs) constituyen fuentes de luz versátiles y apropiadas para todas las aplicaciones mencionadas anteriormente. La longitud de En el régimen ultrarápido, hemos demostrado una nueva técnica de interferometría para la optimización absoluta de la potencia de salida de un oscilador óptico con una cavidad de anillo. Como demostración de principio, implementamos, por primera vez, un OPO de picosegundos en el mid-IR basado en MgO:PPLN con una cavidad de anillo bombeado por un láser de fibra de Yb. Además, hemos desarrollado un nuevo OPO de alta energía en el mid-IR basado en el material nolineal CSP. Esto representa la primera demostración de un OPO compacto de alta repetición sincrónicamente bombeado por un láser de estado sólido a 1064 nm generando pulsos de milijulios en el rango espectral 6-6.5 m. Esta radiación es importante para aplicaciones en cirugía. Adicionalmente, hemos demostrado una fuente verde, 532 nm, basada en láseres de fibra. Esta radiación se obtiene por medio de la generación de segundo harmónico (SHG) en un paso individual en MgO:sPPLT. Esto representa una nueva alternativa de bombeo para los láseres de Ti:sapphire que los harán compactos en el futuro. Los esfuerzos para mejorar la eficiencia de segundo harmónico resultaron en el desarrollo de un novedoso esquema que utiliza múltiples cristales y permite eficiencias de SHG de paso individual del 56%. Este esquema es general y simple y puede ser implementado para cualquier longitud de onda. onda de un OPO puede ser sintonizada en regiones amplias del espectro cambiando la temperatura del cristal no-lineal, el ángulo de ajuste de fase o, al considerar materiales cuasi ajuste de fase (QPM), cambiando el periodo de red. En esta tesis, hemos demostrado una gran variedad de OPOs en el mid-IR en régimen continuo y de pulsos de picosegundo. Estos OPOs han sido bombeados por láseres de fibra permitiendo un diseño compacto y resistente. En el régimen de emisión continua, hemos implementado un OPO de alta potencia basado en MgO:PPLN bombeado por un láser de fibra. Este OPO es sintonízable en el rango 1506-1945 nm correspondiente al infrarrojo-cercano y en el rango 2304-3615 nm correspondiente al mid-IR. Esta capacidad de sintonización se logra al sobrepasar eficientemente los efectos térmicos optimizando el acoplamiento de salida. Materiales nuevos como el MgO:sPPLT, con propiedades ópticas y térmicas mejoradas para la generación de radiación continua en el mid-IR han sido estudiados. Utilizando las propiedades ajuste de la fase extendió del MgO:sPPLT, fuentes continuas de alta potencia con un gran ancho de banda en el infrarrojo-medio también han sido implementadas.

In this thesis the use of high spatial- and spectral-quality diode-laser pump sources for solid-state lasers and continuous-wave optical parametric oscillators (cw OPOs) is investigated. While diode lasers are potentially attractive, compact, low-cost pump sources for solid-state lasers and cw OPOs, the difficulty in obtaining moderate output powers, while retaining high spatial beam quality and spectral purity, often limits the potential of such lasers in these applications. Techniques for obtaining high-power, high spatial- and spectral-quality output from diode lasers are reviewed and the design, development and characterisation of an injection-locked broad-area diode-laser system is described. This system produced output powers of &ap;400mW in a near-diffraction-limited beam (M2&ap;w1.3) and with a spectral width of < 30MHz. The injection-locked system was used as the pump source for a quasi-three-level 946-nm Nd:YAG laser. End-pumped solid-state lasers of this type can offer potentially efficient, low-threshold operation if a near-diffraction limited pump source is used allowing optimal overlap with the laser mode. A model, including pump beam quality effects, is developed for such lasers and used to highlight the advantages of a near- diffraction-limited pump source, especially in the case of the 946-nm Nd:YAG transition which suffers from low gain and significant reabsorption losses. A 946-nm Nd: YAG laser pumped by the injection-locked system is described, yielding cw output powers up to 120mW with a 46% slope efficiency, performance comparable to Ti:sapphire- or dye-laser pumping, and 27ns Q-switched pulses having peak powers of 180W. 50W, 20ns pulses at 473nm were obtained by second-harmonic generation in KNbOs. The performance and relative merits of various cw OPO configurations, in the context of diode-laser pumping, are discussed and the development of a doubly- resonant OPO (DRO) based on periodically-poled lithium niobate is described. When pumped by the injection-locked system, this device showed a threshold of 25mW and .tuning of the outputs over 1.15- 1.25 mum at the signal and 2.3-2.65 mum at the idler was obtained by variation of crystal temperature, PPLN grating period and pump wavelength. When pumping with a 100mW single-mode diode laser, a 15mW OPO threshold was observed while retaining a similar tuning range. This represented the first demonstration of a cw DRO directly pumped by a single-mode diode laser. The achievement of such spectral coverage while pumping with this source points to the potential of such systems as compact, tunable sources in the near-to mid-infrared.

High-power, continuous-wave (cw) optical parametric oscillators (OPOs), from the ultraviolet (UV) and visible to the near- and mid-infrared (IR) wavelength range, are of interest for a variety of applications such as spectroscopy, trace-gas detection and remote sensing. As such, it is desired to investigate OPOs and different frequency conversion techniques, to cover the spectral regions that are inaccessible to lasers, and that too in a compact and low-cost design. This thesis presents the development of high-power cw OPOs, and frequency conversion sources, spanning the UV to mid-IR spectral range, employing different designs, experimental configurations and nonlinear crystals, making them compact and cost-effective. Commercial high-power cw lasers at 1940 nm, 1064 nm and 532 nm have been exploited as the pump sources, in the work presented in this thesis. We have demonstrated a fiber-based cw source at 970 nm, in a simple and practical design. Using direct single-pass second-harmonic-generation (SHG), 13.1 W of output power at 970 nm has been generated in a high-beam-quality, narrow-linewidth, linearly-polarized beam. Further, a technique based on the use of an antiresonant ring (ARR) interferometer for the attainment of optimum output coupling in a cw singly-resonant OPO has been investigated. The technique was deployed in a Yb-fiber-laser-pumped cw OPO based on MgO:PPLN. To extend the tunability of the 1-µm-pumped OPO from the mid-IR to near-IR, SHG of the intracavity signal has been performed in fanout-grating MgO:sPPLT. This compact cw source, tunable across 775¿807 nm, provides >3 W of near-infrared power across 56% of SHG tuning range, in high spatial beam quality. We have also generated output in the UV, down to 355 nm, using single-pass configuration based on sum-frequency-generation of fundamental at 1064 nm and the generated SHG at 532 nm, in BiB3O6. Further, we demonstrated an architecture comprising two cw OPOs coupled together with an ARR interferometer, generating two pairs of signal and idler wavelengths, that can be independently and arbitrarily tuned to indefinitely close spacing, through degeneracy, and beyond, across the wavelength range of 870-1370 nm. The OPOs, based on identical MgO:sPPLT crystals, were pumped by a single cw laser at 532 nm. On the other hand, we also demonstrated active mode-locking of cw OPOs using direct low-frequency electrooptic phase-modulation (EOM), opening up the possibility of avoiding the need for ultrafast laser sources and synchronous pumping. We have generated picosecond pulses in doubly- and singly-resonant configuration. Also, a technique based on the deployment of the EOM in combination with an ARR interferometer internal to the cw OPO has been investigated for active modelocking.

This thesis describes an experimental investigation of optical frequency conversion in isotropic semiconductor waveguides by use of several phase-matching approaches. Efficient, type I second harmonic generation of femtosecond pulses is reported in birefringently-phase-matched GaAs/Alox waveguides pumped at 2.01 μm. Practical second harmonic average powers of up to ~ 650 μW are obtained, for an average launched pump power of ~ 5 mW. This corresponds to a waveguide conversion efficiency of ~ 20 % and a normalized conversion efficiency of greater than 1000 % W−1cm−2. Pump depletion of more than 80 % is recorded. Second harmonic generation by type I, third order quasi-phase-matching in a GaAs- AlAs superlattice waveguide is reported for fundamental wavelengths from ~1480 to 1520 nm. Quasi-phase-matching is achieved through modulation of the nonlinear coefficient χ[sub](zxy)(2), which is realised by periodically tuning the superlattice bandgap. An average output power of ~25 nW is obtained for a launched pump power of < 2.3 mW. Type I second harmonic generation by use of first order quasi-phase-matching in a GaAs/AlAs symmetric superlattice waveguide is also reported, with femtosecond fundamental pulses at 1.55 μm. A periodic spatial modulation of the bulk-like second- order susceptibility χ[sub](zxy)(2) is realized using quantum well intermixing by As+ ion implantation. A practical second harmonic average power of ~1.5 μW is detected, for a coupled pump power of ~11 mW. Second harmonic generation through modal-phase-matching in GaAs/AlGaAs semiconductor waveguides is reported. Using femtosecond pulses, both type I and type II second harmonic conversion is demonstrated for fundamental wavelengths near 1.55 μm. An average second harmonic power of ~10.3 μW is collected at the waveguide output for a coupled pump power of < 20 mW. For a complete characterisation, the optical loss is measured in these nonlinear GaAs- based waveguides over the spectral range 1.3-2.1 μm in the infrared, by deploying a femtosecond scattering technique. Typical losses of ~5-10 dB/cm are measured for the best of the waveguides, while a systematic intensity and wavelength dependent study revealed the contribution of Rayleigh scattering and two photon absorption in the overall transmission loss.