<p>This thesis explores the use of nonlinear crystals from theKTiOPO₄(KTP) family with the aim to extend the possibleapplications for laser sources and to gain more knowledge aboutthe material’s benefits and limits. The work focussed onoptical parametric oscillators (OPOs) and optical parametricamplifiers (OPAs), which employ second order nonlinearprocesses. Both devices transfer energy from a laser beam at aparticular wavelength to a different wavelength, which istuneable. In OPOs two new beams at different wavelengths aregenerated, whereas in OPAs an existing weak beam is amplified.The essential part of these devices, which enables theoccurrence of the energy conversion, is a nonlinear crystal. Inthis work the ferroelectric crystals KTP and RbTiOPO₄(RTP) have been utilized.</p><p>By modifying the material’s structure,quasi-phasematching can be obtained, which is a crucialrequirement for achieving efficient energy conversion betweenthe incident and the generated waves. The fabrication ofquasi-phasematched crystals is dependent on the controlledreversion of the material’s spontaneous polarisation,which is accomplished by periodic electric field poling.</p><p>Nanosecond pulses of more than 200 kW were generated in the“eye-safe”region by employing a double pass OPA.Small signal gains exceeding 75 dB were obtained for anessentially diffraction limited beamwithout spectralbroadening of the seed. By subsequent signal coupling intofibres substantial broadening was accomplished. A systematicmeasurement series of several RTP crystals allowed us toaccurately determine the wavelength and temperature dispersionof the refractive index, which are two essential requirementsfor further employment of this material. The OPOs based on RTPwere widely tuneable by controlling the temperature. It wasalso concluded that RTP behaves similar to KTP in parametricdevices, thus being a material, which can sustain high powers,possesses large nonlinear coefficients and can operate in abroad wavelength region.Efficient Raman oscillation concurrent with parametricoscillation was observed and analysed in several KTP samples.This gave further insight into the processes taking placeinside the material when performing as a frequency converter,if the generated idler lies in the absorption band.This thesis also covers the investigation of afemtosecond optical parametric chirped pulse amplifier.Temporally stretched seed pulses were amplified to 85 µJ,resulting in a gain above 60 dB, and subsequent recompressionresulted in 270 fs pulses.</p><p><b>Keywords:</b>nonlinear optics, KTiOPO₄, optical parametric oscillator, optical parametricamplifier, RbTiOPO₄, quasi-phasematching, electric field poling,stimulated Raman scattering.</p>

This thesis explores the use of nonlinear crystals from theKTiOPO4(KTP) family with the aim to extend the possibleapplications for laser sources and to gain more knowledge aboutthe material’s benefits and limits. The work focussed onoptical parametric oscillators (OPOs) and optical parametricamplifiers (OPAs), which employ second order nonlinearprocesses. Both devices transfer energy from a laser beam at aparticular wavelength to a different wavelength, which istuneable. In OPOs two new beams at different wavelengths aregenerated, whereas in OPAs an existing weak beam is amplified.The essential part of these devices, which enables theoccurrence of the energy conversion, is a nonlinear crystal. Inthis work the ferroelectric crystals KTP and RbTiOPO4(RTP) have been utilized. By modifying the material’s structure,quasi-phasematching can be obtained, which is a crucialrequirement for achieving efficient energy conversion betweenthe incident and the generated waves. The fabrication ofquasi-phasematched crystals is dependent on the controlledreversion of the material’s spontaneous polarisation,which is accomplished by periodic electric field poling. Nanosecond pulses of more than 200 kW were generated in the“eye-safe”region by employing a double pass OPA.Small signal gains exceeding 75 dB were obtained for anessentially diffraction limited beamwithout spectralbroadening of the seed. By subsequent signal coupling intofibres substantial broadening was accomplished. A systematicmeasurement series of several RTP crystals allowed us toaccurately determine the wavelength and temperature dispersionof the refractive index, which are two essential requirementsfor further employment of this material. The OPOs based on RTPwere widely tuneable by controlling the temperature. It wasalso concluded that RTP behaves similar to KTP in parametricdevices, thus being a material, which can sustain high powers,possesses large nonlinear coefficients and can operate in abroad wavelength region.Efficient Raman oscillation concurrent with parametricoscillation was observed and analysed in several KTP samples.This gave further insight into the processes taking placeinside the material when performing as a frequency converter,if the generated idler lies in the absorption band.This thesis also covers the investigation of afemtosecond optical parametric chirped pulse amplifier.Temporally stretched seed pulses were amplified to 85 µJ,resulting in a gain above 60 dB, and subsequent recompressionresulted in 270 fs pulses. <b>Keywords:</b>nonlinear optics, KTiOPO4, optical parametric oscillator, optical parametricamplifier, RbTiOPO4, quasi-phasematching, electric field poling,stimulated Raman scattering. / NR 20140805

This thesis deals with the fabrication and the characterization of periodically-poled crystals for use in lasers to generate visible and UV radiation by second-harmonic generation (SHG) through quasi-phasematching (QPM). Such lasers are of practical importance in many applications like high-density optical storage, biomedical instrumentation, colour printing, and for laser displays. The main goals of this work were: (1) to develop effective monitoring methods for poling of crystals from the KTiOPO4 (KTP) family, (2) to develop useful non-destructive domain characterization techniques, (3) to try to find alternative crystals to KTP for easier, periodic poling, (4) to investigate the physical mechanisms responsible for optical damage in KTP. The work shows that the in-situ SHG technique used together with electro-optic monitoring, makes it possible to obtain reliable, real-time information regarding the poling quality over the whole crystal aperture during the electric-field poling process. Using this combined monitoring method, both KTP and Rb-doped KTP (RKTP) crystals were successfully poled. By comparing these two crystals, we found that a low-doped KTP has a substantially reduced ionic conductivity and, thus, a high-quality periodic poling can be obtained without otherwise affecting the properties of the crystal. RKTP is a good alternative candidate to KTP for poling purpose. We have also shown that Atomic Force Microscopy (AFM) is an informative tool for investigating domain nucleation, growth, and merging. Furthermore, we have demonstrated a simple technique for 3D characterization of QPM samples. It utilizes a group-velocity mismatched, type-II SHG of femtosecond pulses for layer-by-layer monitoring of the effective nonlinearity along the propagation direction of the beam. The quality of these crystals was finally reflected in a number of SHG experiments with a variety of laser sources. High energies and high efficiencies were thus demonstrated using CW, mode-locked and Q-switched lasers. Gratings with pitches smaller than 3 µm, were demonstrated for first-order UV generation. Type-II QPM SHG was demonstrated as a technique for reducing the fabrication constraints. High intensity light in the visible and the UV leads to modification of the material properties and, eventually, to optical damage. In KTP and its isomorphs, the first sign of material change is an optically-induced absorption. We have used thermal-lens spectroscopy with a common-path interferometer for high-sensitivity measurements of green light-induced infrared absorption dynamics in single-domain and periodically-poled KTP (PPKTP). The saturated, green light-induced absorption has been shown to be consistently higher in periodically-poled crystals, and is attributed to the creation of stoichiometric and interstitial defects in the crystals during the poling process. Finally, irreversible bulk damage thresholds in PPKTP have been determined for pulsed frequency converters. As the characteristics of optical damage are closely related to the material quality, this investigation can provide useful information for crystal manufactures and will help to optimise the crystal growth conditions.

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. 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). 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. 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. <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.

Ferroelectric crystals are commonly used in nonlinear optics for frequency conversion of laser radiation. The quasi-phase matching (QPM) approach uses a periodically modulated nonlinearity that can be achieved by periodically inverting domains in ferroelectric crystals and allows versatile and efficient frequency conversion in the whole transparency region of the material. KTiOPO4 (KTP) is one of the most attractive ferroelectric non-linear optical material for periodic domain-inversion engineering due to its excellent non-linearity, high resistance for photorefractive damage, and its relatively low coercive field. A periodic structure of reversed domains can be created in the crystal by lithographic patterning with subsequent electric field poling. The performance of the periodically poled KTP crystals (PPKTP) as frequency converters rely directly upon the poling quality. Therefore, characterization methods that lead to a deeper understanding of the polarization switching process are of utmost importance. In this work, several techniques have been used and developed to study domain structure in KTP, both in-situ and ex-situ. The results obtained have been utilized to characterize different aspects of the polarization switching processes in KTP, both for patterned and unpatterned samples. It has also been demonstrated that it is possible to fabricate sub-micrometer (sub-μm) PPKTP for novel optical devices. Lithographic processes based on e-beam lithography and deep UV-laser lithography have been developed and proven useful to pattern sub- μm pitches, where the later has been the most convenient method. A poling method based on a periodical modulation of the K-stoichiometry has been developed, and it has resulted in a sub-μm domain grating with a period of 720 nm for a 1 mm thick KTP crystal. To the best of our knowledge, this is the largest domain aspect-ratio achieved for a bulk ferroelectric crystal. The sub-micrometer PPKTP samples have been used for demonstration of 6:th and 7:th QPM order backward second-harmonic generation with continuous wave laser excitation, as well as a demonstration of narrow wavelength electrically-adjustable Bragg reflectivity. / QC 20100930

<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 deals with the fabrication and the characterization of periodically-poled crystals for use in lasers to generate visible and UV radiation by second-harmonic generation (SHG) through quasi-phasematching (QPM). Such lasers are of practical importance in many applications like high-density optical storage, biomedical instrumentation, colour printing, and for laser displays.</p><p>The main goals of this work were: (1) to develop effective monitoring methods for poling of crystals from the KTiOPO₄ (KTP) family, (2) to develop useful non-destructive domain characterization techniques, (3) to try to find alternative crystals to KTP for easier, periodic poling, (4) to investigate the physical mechanisms responsible for optical damage in KTP. The work shows that the in-situ SHG technique used together with electro-optic monitoring, makes it possible to obtain reliable, real-time information regarding the poling quality over the whole crystal aperture during the electric-field poling process. Using this combined monitoring method, both KTP and Rb-doped KTP (RKTP) crystals were successfully poled. By comparing these two crystals, we found that a low-doped KTP has a substantially reduced ionic conductivity and, thus, a high-quality periodic poling can be obtained without otherwise affecting the properties of the crystal. RKTP is a good alternative candidate to KTP for poling purpose. We have also shown that Atomic Force Microscopy (AFM) is an informative tool for investigating domain nucleation, growth, and merging. Furthermore, we have demonstrated a simple technique for 3D characterization of QPM samples. It utilizes a group-velocity mismatched, type-II SHG of femtosecond pulses for layer-by-layer monitoring of the effective nonlinearity along the propagation direction of the beam. The quality of these crystals was finally reflected in a number of SHG experiments with a variety of laser sources. High energies and high efficiencies were thus demonstrated using CW, mode-locked and Q-switched lasers. Gratings with pitches smaller than 3 µm, were demonstrated for first-order UV generation. Type-II QPM SHG was demonstrated as a technique for reducing the fabrication constraints.</p><p>High intensity light in the visible and the UV leads to modification of the material properties and, eventually, to optical damage. In KTP and its isomorphs, the first sign of material change is an optically-induced absorption. We have used thermal-lens spectroscopy with a common-path interferometer for high-sensitivity measurements of green light-induced infrared absorption dynamics in single-domain and periodically-poled KTP (PPKTP). The saturated, green light-induced absorption has been shown to be consistently higher in periodically-poled crystals, and is attributed to the creation of stoichiometric and interstitial defects in the crystals during the poling process. Finally, irreversible bulk damage thresholds in PPKTP have been determined for pulsed frequency converters. As the characteristics of optical damage are closely related to the material quality, this investigation can provide useful information for crystal manufactures and will help to optimise the crystal growth conditions.</p>

Lithium niobate (LiNbO3) and KTiOPO4 (KTP) are ferroelectric crystals of considerable interest in different fields of optics and optoelectronics. Due to its large values of the nonlinear optical, electro-optic (EO), piezoelectric and acousto-optical coefficients, LiNbO3 is widely used for laser frequency conversion using the quasiphase matching (QPM) approach where the sign of nonlinearity has been periodically modulated by electric field poling (EFP). In the microwave and telecommunication field LiNbO3 is used for surface acoustic devices and integrated optical modulators. KTP and its isomorphs, on the other hand, exhibit slightly lower nonlinear coefficients but have much higher photorefractive damage thresholds, so that it is mainly used in the fabrication of QPM devices for both UV, IR and visible light generation and in high power applications. This thesis focus on different key issues: (1) accurate characterization of specific optical properties of LiNbO3, which are of interest in nonlinear and EO applications; (2) in-situ visualization and characterization of domain reversal by EFP in LiNbO3 and KTP crystals for a through understanding of the ferroelectric domain switching; (3) fabrication of periodic surface structures at sub-micron scale in LiNbO for photonic applications. An interferometric method is used for accurate measurement of ordinary and extraordinary refractive indices in uniaxial crystals, which is of great interest in the proper design of QPM crystals. A digital holography (DH) based method is presented here for 2D characterization of the EO properties of LiNbO , which is considerably interesting in the applications where the proper design of the EO device requires a spatially resolved information about the EO behaviour and the existing pointwise techniques are not sufficient. A DH method for novel in-situ monitoring of domain reversal by EFP in both LiNbO3 and KTP, is also presented here. The technqiue could be used as a tool for high fidelity periodic domain engineering but also provides information about domain kinetics, internal field and crystals defects. 3 3 3 Finally this thesis presents novel results concerning nanoscale periodic surface structuring of congruent LiNbO3. Holographic lithography (HL) is used for sub-micron period resist patterning and electric overpoling for surface domain reversal. Surface structures are obtained by selective etching. Moiré effect is also used in the HL to fabricate complicated structures with multiple periods. The depth compatibility with waveguide implementation allows foreseeing possible applications of these structures for Bragg gratings or innovative photonic crystal devices, exploiting the additional nonlinear and EO properties typical of LiNbO3. / QC 20100824

Nonlinear optical frequency conversion is one of the most important key techniques in order to obtain lasers with wavelengths targeted for specific applications. In order to realize efficient and tailored lasers, the quasi-phase-matching (QPM) approach using periodically-poled ferroelectric crystals is getting increasingly important. Also understanding of damage mechanisms in nonlinear materials is necessary to be able to design reliable and well working lasers. This is especially true for high power application lasers, which is a rapidly growing field, where the damage problem normally is the ultimate limiting factor. In this thesis work, several promising novel ferroelectric materials have been investigated for nonlinear optical applications and the emphasis has been put on QPM devices consisting of periodically-poled structures. The materials were selected from three different types of ferroelectric materials: 1) MgO-doped stoichiometric LiNbO3 (MgO:SLN) and LiTaO3 (MgO:SLT), and non-doped stoichiometric LiTaO3 (SLT), 2) KTiOPO4 (KTP) and its isomorphs RbTiOPO4 (RTP), and 3) KNbO3 (KN). The focus in our investigations have been put on the spontaneous polarization switching phenomena, optimization of the periodic poling conditions, and the photochromic optical damage properties which were characterized by the help of blue light-induced infrared absorption (BLIIRA) measurements. With electrical studies of the spontaneous polarization switching, we were able to determine quantitatively, and compare, the coercive field values of different materials by applying triangularly shaped electric fields. We found that the values of the coercive fields depended on the increase rate of the applied electric field. The coercive field of KN was the lowest (less than 0.5 kV/mm) followed by the ones of KTP, SLT, and MgO:SLT (1.5 to 2.5 kV/mm). MgO:SLN, and RTP had relatively high coercive fields, approximately 5.0 to 6.0 kV/mm, respectively. Based on the domain switching characteristics we found, we successfully fabricated periodically-poled devices in all of the investigated materials with 30 μm periodicities and sample thickness of 1 mm. Blue light-induced infrared absorption (BLIIRA) has been characterized for unpoled bulk and periodically-poled samples using a high-sensitivity, thermal-lens spectroscopy technique. SLT showed a large photorefraction effect and the BLIIRA signal could not be properly measured because of the large distortion of the probe beam. The rise and relaxation time of BLIIRA, after switching the blue light on and off was in a time span of 10 to 30 sec except for KTP and its isomorphs, which needed minutes to hours in order to saturate at a fixed value. KN and MgO:SLN showed the lowest susceptibility to the induced absorption. Periodic poling slightly increased the susceptibility of KTP, MgO:SLT, and KN. Relatively high thresholds were observed in MgO:SLT and KN. By increasing the peak-power intensity of the blue light, the induced absorption for MgO:SLN, KTP and KN saturated at a constant value while that of MgO:SLT increase in a constant fashion. This trend is critical issue for the device reliability at high-power applications. / QC 20100830

Amorphous materials present macroscopic inversion symmetry. As a consequence, their even order nonlinearities are null. The technological interest in vitreous medium with second order nonlinearity ( &#967;(2) ) to make photonic devices has stimulated the development of techniques to induce this property. Among them, the thermal-electric field poling is one of the most investigated due its experimental simplicity and results reproducibility. In this work the investigations were directed to the thermal-electric field poling dynamics in soda-lime glasses in view of identify the mainly contributions to the induced nonlinearity stability. Initially were identified the mainly contributions to the induced electrical current. It was observed during the polarizations electroluminescence emission which was shown to be due to ionic displacement and air ionization outside the sample. By using a simplified ionic conduction model was determined two activation energies: ~0,60 and ~3,8eV. The first one, determined from the induced electrical current, was attributed to the sodium conduction; while the second ones, determined by the electroluminescence, attributed to the calcium displacement. Besides the small contribution to the electrical current, the calcium ions, due their small diffusion coefficient, were identified as responsible to the possibility of induce stable second order nonlinearity in soda-lime glasses. Based on these evidences it was used an alternative procedure in which the electrical current flux is controlled. This procedure enabled induce stable &#967;(2) . This effect was demonstrated to exist 12 months after the polarization procedure, even with a ~50% decrease. The second harmonic generation efficiency was increased in until three times by pumping continuously the polarized samples with infrared radiation from an Nd-YAG laser operating at QSML regime. The threshold applied voltage to observe &#967;(2) was determined through a modulated applied voltage procedure to be due to the mobility difference between sodium and calcium. / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / Materiais amorfos apresentam simetria de inversão macroscópica e, como conseqüência, as nãolinearidades ópticas de ordem par são nulas. A necessidade tecnológica de que meios vítreos apresentem não-linearidade de segunda ordem ( &#967;(2) ), visando principalmente o desenvolvimento de dispositivos fotônicos, fortalece a busca por técnicas para a sua indução. Dentre estas, o processo termo-elétrico de polarização tem sido muito investigado devido, principalmente a sua simplicidade experimental e a reprodutibilidade dos resultados. Neste trabalho as investigações são dedicadas à dinâmica do processo termo-elétrico em vidros soda-lime visando identificar as principais contribuições para a estabilidade da não-linearidade induzida. Inicialmente foram verificadas as principais contribuições à corrente elétrica induzida. Durante as polarizações observou-se emissão de eletroluminescência. Mostrou-se que esta é devido ao deslocamento dos íons de cálcio e possíveis ionizações do ar fora da amostra. Usando um modelo simplificado de condução iônica determinou-se duas energias de ativação: ~0,60 e ~3,8eV. A primeira, determinada a partir da corrente elétrica induzida, foi atribuída à condução dos íons de sódio; enquanto a segunda, determinada pela eletroluminescência, aos íons de cálcio. Apesar de pequena contribuição na corrente elétrica induzida, os íons de cálcio, devido ao baixo coeficiente de difusão, foram identificados como os responsáveis pela possibilidade de indução de &#967;(2) estável em vidros soda-lime. Baseado nessas evidências foi utilizado um procedimento alternativo de polarização controlando do fluxo de corrente induzida que permitiu a indução de &#967;(2) estável. Este efeito pôde ser comprovado existir 12 meses após o processo de polarização, mesmo com redução de ~50% do valor inicial. Observou-se que a eficiência na geração de segundo harmônico pôde ser aumentada em até 3 vezes quando as amostras polarizadas foram bombeadas continuamente com laser Nd-YAG operando no regime QSML. Através de procedimento com tensão elétrica aplicada modulada foi identificada a origem da tensão elétrica de limiar como sendo devido à diferença de mobilidade entre os íons de sódio e cálcio.