Cette thèse porte sur l'élaboration de céramiques transparentes de CaF2 :Yb pour la réalisation de milieux amplificateurs pour laser de puissance. Dans ce domaine, les céramiques laser constituent une rupture technologique en palliant les limites des matériaux actuels - monocristaux (problèmes de dimensions accessibles) et verres (mauvaises propriétés thermiques). L'originalité du travail est de s'intéresser aux fluorures, très attractifs pour leur faible fréquence de phonons et leur large fenêtre de transparence spectrale. Trois synthèses de nanoparticules de CaF2 :Yb ont été mises au point : la mécanosynthèse, la méthode par micelles inverses et la précipitation. Après caractérisation microstructurale des poudres, la précipitation a été retenue : elle est simple et les particules répondent aux critères fixés (taille moyenne ~30 nm, faible dispersion en taille

Various experiments on Yb₂Ti₂O₇ have shown evidence of strange magnetic behaviour at low temperatures. Specific heat measurements on powder samples of Yb₂Ti₂O₇ show evidence of a sharp peak, indicating the occurence of a first order phase transition. Meanwhile, neutron scattering, Mössbauer absorption, and μSR measurements find no evidence of long range order below the temperature of this phase transition, leaving the nature of the low temperature phase a mystery. Quantifying the magnetic interactions in this material should allow us to better understand the low temperature behaviour of this material. In this study, we fit a symmetry allowed nearest-neighbour bilinear exchange model to quasi-elastic neutron scattering data collected well above the temperature of the experimentally observed phase transition. This neutron scattering data shows evidence of rods of scattering intensity along the ⟨111⟩ crystallographic directions. Neutron scattering probes the correlations between magnetic moments in a material, so fitting an interaction model to the neutron scattering is equivalent to fitting the interactions to the magnetic correlations. These correlations are driven by the interactions between the magnetic moments, so the neutron scattering should give us direct access to the form of these interactions. Using this method we successfully identify an anisotropic nearest-neighbour bilinear exchange model that reproduces the experimentally observed quasi-elastic neutron scattering. With this model we then proceed to compute real space correlation functions, finding that the rods of neutron scattering arise from the presence of strong correlations along nearest-neighbour chains. We also compute the bulk susceptibility and local susceptibility, obtaining very good fits to experiment with no variation of the model determined from the neutron scattering. The success of these calculations provides a further independent confirmation of the success of our interaction model in describing the magnetic interactions in Yb₂Ti₂O₇. Finally, we present a brief summary of ongoing work based on our anisotropic exchange model, including mean field calculations to determine the low temperature ground state of this model and classical Monte Carlo simulations to study the phase transition present in this model. We also discuss potential further studies of this and other models.

Due to the fast expansion and development in the optical communication industry, the demand for the broad-band laser light source as used to the optical transmission network system has correspondingly increased. Cr4+ doped YAG crystal fibers, with its broad-band spectral property, is thus becoming more and more indispensable to the growth of the industry. However, the Cr4+:YAG crystal fiber in its own repetitive growth process brings with itself one problem: after each re-growth, the concentration of Cr2O3 and Cr4+ ions would reduce appreciatively. Hence, finding sound solutions for effectively raising the concentration of Cr4+ is now becoming an essential issue in the field. The thesis mainly focuses on the development of using Cr4+:YAG as the laser gain medium. Thin layers of CaO, MgO, and Cr2O3 was coated on the circumference of the Cr:YAG crystal fiber. The LHPG method was then employed to re-grow the coated samples, during which the doped concentration of CaO, MgO and Cr2O3 can in-diffuse. And the effect of charge compensation would go further to simultaneously raise the concentration of Cr4+ ions. Now we have successfully enhance the concentration of Cr4+ ions to 4.86x10-3 wt.%. This study, with the use of the E-Gun coating machine and the IAD (ion-beam assisted deposition) system, also probes the technical side of how to better improve the quality of the crystal fiber laser. Both end faces of the Cr4+:YAG crystal fiber were coated with optical thin films by TiO2 and SiO2 targets. In addition to raise the quality of the thin films, the IAD system also functions to create a laser cavity in which both the anti-reflectance (AR) effect (for pumping the light source) and the high reflectance (HR) effect (for stimulating the light source) are achieved. The accompanied benefits would be the reduction of transmission loss, the increased laser efficiency, and thus a more successful and more stable crystal fiber laser.

The research presented in this dissertation was performed in the Atomic, Molecular and Optical (AMO) physics laboratory at the University of Manitoba. Atomic beams of the two-valence-electron heavy atom systems, barium and ytterbium, were investigated with low energy electron scattering and optical emission studies. Both the ground states and laser excited states were investigated as a function of incident electron beam energy from 10 eV to 50 eV. Measurements of relative cross sections and polarization for 583 nm and 554 nm line emission from the (6s7p)1P1 and (6s6p)1P1 states of barium excited by electron impact from both the ground states and the optically pumped metastable (6s5d)1D2 are reported. Data are normalized to absolute cross sections for the ground state (6s2)1S0→(6s6p)1P1 state transition due to electron scattering, with corrections for branching ratios and cascading from higher states to deduce the total level excitation cross sections. Results are also presented for the first studies of the 399 nm line emission from laser-excited ytterbium, yielding an upper limit on the apparent cross section for the (6s6p)3P1→(6s6p)1P1 transition. Results are compared with the latest theoretical models and previous data, where available. / October 2015

In this thesis, I have developed a tunable two-color two-stage ultrafast Yb:fiber chirped pulse amplifier for the generation of short-pulse mid-infrared (MIR) radiation in the long-wavelength side of the "molecular fingerprint" (2.5-25 μm) using difference frequency generation (DFG) technique. The two colors called blue and red are in the wavelengths 1.03-1.11 μm and are amplified simultaneously in the same Yb-doped fiber amplifier (YDFA) stages in order to reduce the induced environmental noise on the phase difference of the pulses and to minimize the complexity and system cost. I will present numerical simulations on the two-stage YDFA system to amplify a two-color spectrum in the wavelengths 1.03-1.11 μm. The first and second YDFA called preamplifier and main amplifier are single-clad, single-mode and double-clad, single-mode YDFA respectively. From numerical simulations, the optimal length of the preamplifier to have equal power at two colors centered at 1043 nm and 1105 nm are in agreement with experimental results. It is well known that the power of MIR radiation generated by difference frequency mixing of two wavelengths scales up with the product of mixing powers in a fixed-field approximation. Furthermore, for the gain narrowing effect on the short-wavelength side of the YDFA gain profile, the spectral bandwidth of the blue color decreases resulting in pulse broadening. In addition, for the two colors separated largely, the amplified spontaneous emission is intensified. Considering the cited factors, I will present the modeling results on the two-color, two-stage YDFA system that the product of the power of the two colors is maximized for a maximized wavelength separation between the two mixing colors and a minimized gain narrowing on the blue color in order to build an as broadly tunable and powerful as possible ultrafast mid-infrared source by difference frequency mixing of the two colors. In this research, I achieved a wavelength separation as broad as 71 nm between pulses centered at 1038 nm and 1109 nm from the two-color ultrafast YDFA system. I achieved combined average powers of 2.7 W just after the main amplifier and 1.5 W after compressing the two-color pulses centered at 1041 nm and 1103 nm to nearly Fourier transform limited pulses. From autocorrelation measurements, the full width at half maximum (FWHM) of the compressed two-color pulses with the peak wavelengths of 1041 nm and 1103 nm was ~500 fs. By mixing the tunable two-color pulses in a 1-mm-thick GaSe crystal using DFG technique, I achieved tunable short-pulse MIR radiation. In this research, I achieved short-pulse MIR radiation tunable in the wavelengths 16-20 μm. The MIR tuning range from the lower side was limited to the 16 μm because of the 71-nm limitation on the two-color separation and from the upper side was limited to the 20 μm because of the 20-μm cutoff absorption wavelength of GaSe. Based on measured MIR spectra, the MIR pulses have a picosecond pulse duration in the wavelengths 16-20 μm. The FWHM of measured spectra of the MIR pulses increases from 0.3 μm to 0.8 μm as the MIR wavelength increases from 16 μm to 20 μm. According to Fourier transform theory, the FWHM of the MIR spectra corresponds to the bandwidth of picosecond MIR pulses assuming that the MIR pulses are perfectly Fourier-transform-limited Gaussian pulses. In this research, I achieved a maximum average power of 1.5 mW on short-pulse MIR radiation at the wavelength 18.5 μm corresponding to the difference frequency of the 500-fs two-color pulses with the peak wavelengths of 1041 nm and 1103 nm and average powers of 1350 mW and 80 mW respectively. Considering the gain bandwidth, Ti:sapphire is a main competitor to the YDFA to be used in the two-color ultrafast laser systems. In the past, the broad gain bandwidth of Ti:sapphire crystal has resulted in synchronized two-color pulses with a wavelength separation up to 120 nm. Apart from its bulkiness and high cost, Ti:sapphire laser system is limited to a watt-level output average power at room temperature mainly due to Kerr lensing problem that occurs at high pumping powers. In comparison, YDFA as a laser amplifier has a narrower gain bandwidth but it is superior in terms of average power. Optical parametric generation (OPG) and optical parametric amplification (OPA) techniques are two competitors to DFG technique for the generation of short-pulse long-wavelength MIR radiation. Although OPG offers a tunability range as broad as DFG, the MIR output power is lower because of the absence of input signal pulses. From the OPA technique, the tunability range is not as broad as the DFG technique due to limitations with the spectral bandwidth of the optical elements. Currently, quantum cascade lasers (QCLs) are the state-of-art MIR laser sources. At the present time, the tunability range of a single MIR QCL is not as abroad as that achieved from the DFG technique. More, mode-locked MIR QCLs are not abundant mainly because of the fast gain recovery time. Thus, the generation of widely tunable short-pulse MIR radiation from DFG technique such as that developed in this thesis remains as a persistent technological solution. The application of the system developed in this thesis is twofold: on one hand, the tunable two-color ultrashort pulses will find applications for example in pump-probe ultrafast spectroscopy, short-pulse MIR generation, and optical frequency combs generation. On the other hand, the short-pulse MIR radiation will find applications for example in time-resolved MIR spectroscopy to study dynamical behavior of large molecules such as organic and biological molecules.

Yb-ion doped gain media have become the material of choice for reliable generation of ultrashort pulses at wavelength around 1 μm. At present, however, operation at high average power (>1 W) with sub-100 fs pulses still remains challenging. The efforts of developing an Yb-ion oscillator towards this goal, therefore, are the main focus of this thesis. In this work, the Yb:KGd(WO4)2 (Yb:KGW) crystals were chosen to serve as the gain media. To achieve high power operation, two fundamental issues have been carefully considered: 1) a new pumping scheme was proposed to alleviate the thermal issues in the Yb:KGW crystals; 2) a new method was introduced to characterize intracavity losses in the broadband Yb-ion oscillators. As a side effect observed during the optimization of the CW operation, simultaneous two-wavelength emission was also discussed. With the knowledge and experimental understanding of the fundamental issues in laser oscillators operated in the continuous-wave regime, the next step of this work demonstrated their operation in a pulsed regime. The dual action of the Kerr-lens and saturable absorber (KLAS) mode locking was proposed in this work and resulted in greatly enhanced laser performance. The laser delivered pulses with 67 fs duration at a repetition rate of 77 MHz. The average output power reached 3 W, which, to the best of our knowledge, is the highest average output power produced to date from the Yb-ion based bulk lasers with such a short pulse duration. The scalability of pulse energy and peak power was also demonstrated by reducing the repetition rate to either 36 MHz or 18 MHz. The cavity with the latter repetition rate produced 85 fs pulses with the pulse energy up to 83 nJ, which corresponds to a peak power as high as 1 MW. As required by many biomedical applications, the wavelength of the generated pulses (~1 μm) can be tuned in the near-infrared region by coupling them into an optical parametric oscillator (OPO). The feasibility of this approach was demonstrated in the last part of this thesis, through a thorough theoretical analysis of two OPO materials suitable for excitation at 1.04 μm.

Horses consume large amounts of fiber in their diet, which may affect digestibility and digesta rate of passage. The objective of these studies was to assess the effects of diet composition on digestibility and rate of passage in horses using mathematical models. Using previously published data, forage dry matter digestibility (DMD) was related to forage neutral detergent fiber (NDF) concentrations and crude protein (CP) concentrations (DMD = 66.1178 – 0.3410*NDF + 0.6356*CP, DM basis; P < 0.001). In a second experiment, horses were fed diets formulated to have high fiber (HF, n= 3; NDF = 55.3%, CP = 11.8%) or low fiber (LF, n = 3; NDF = 40.5%, CP = 13.3%) concentrations. The LF treatment had greater DM, organic matter, and gross energy digestibilities (P < 0.05), whereas the HF treatment had greater NDF digestibility (P < 0.05). Mathematical models were useful to determine mean retention time (MRT) and there were no differences between model MRT and algebraic MRT, or treatment. Some compartmental parameters were different between treatments (P < 0.05), indicating that dietary fiber may alter some components of digesta passage in horses.

The spectroscopy of wide-bandgap fluoride materials doped with divalent ytterbium is presented. The structure of impurity-trapped excitons is explored, vacuum ultraviolet excitation is used to investigate the transfer processes between excitations, and the effect of confinement on self-trapped excitons is studied. The excited-state structure of impurity-trapped excitons is measured in the multisite system NaMgF₃:Yb²⁺. A two-colour ultraviolet-infrared pulsed photoluminescence enhancement technique is employed to probe the interlevel transitions and dynamics of impurity-trapped excitons in doped insulating phosphor materials. NaMgF₃:Yb²⁺ exhibits emission from two charge-compensation centres with peaks at 22 300 cm⁻¹ (448 nm) and 24 000 cm⁻¹ (417 nm). The observed photoluminescence enhancement is caused by a combination of intra-excitonic excitation and electron trap liberation. The electron traps are inferred to have a depth of approximately 800 cm⁻¹. Time-resolved VUV spectroscopic studies of emission and excitation spectra of CaF₂:Yb, NaMgF₃Yb and MgF₂:Yb are presented to investigate excitation and relaxation mechanisms of both impurity-trapped excitons and intrinsic excitons in each fluoride host. Host-to-impurity energy transfer mechanisms leading to formation of impurity-trapped excitons are discussed. The 4f¹⁴ → 4f¹³5d CaF₂:Yb²⁺ absorption bands are successfully modeled with a semi-empirical effective Hamiltonian calculation for NaMgF₃:Yb²⁺ and MgF₂:Yb²⁺. The excitation and emission spectra of all studied materials are compared. Results on VUV spectroscopy of 3 and 5 monolayer CdF₂–CaF₂ superlattices show the change in optical behaviour of the self-trapped exciton in CdF₂ when it is confined and give an indication of the radius of the exciton. The decay of the emission is modeled with three components, corresponding to three self-trapped exciton states. Results on the VUV spectroscopy of CdF₂–CaF₂ superlattices show that the confinement effect seems to equally influence the energy of excitonic and bandgap absorption in 3 and 5 monolayer superlattices. At the same time, as the self-trapped exciton is more confined, the emission is blue-shifted by 1600 cm⁻¹ indicating that the effective excitonic radius is about three monolayers.

Studies have been done to determine rare-earth elements’ optical and luminescent properties using wide bandgap nitride semiconductors as suitable hosts. Research done here will contribute to the information needed to further study rare-earth elements and their unique properties. Thin films of rare-earth elements erbium, terbium, ytterbium, and both erbium and ytterbium doped into AlN are studied by laser excitation. A 532 nm Nd: YAG green laser and 783nm crystal infrared laser are used for excitation in conjunction with a spectrometer to measure photoluminescence. With the 532 nm laser, AlN: Er emits peaks at 554 nm, 561 nm, and 1552 nm, AlN: Tb emits peaks at 549 nm and 562 nm, AlN: Yb emits peaks at 966 nm, and co-doped AlN: ErYb contains peaks including both AlN: Er and AlN: Yb. Energy transfer occurred from Er to Yb resulting in an increased magnitude and peak shift. The 783 nm laser gave peaks at 1563nm for AlN: Er, 1508 nm and 1533 nm for AlN: Tb, and 1567nm for AlN: ErYb. No detectable peaks were given for AlN: Yb. A peak shift was detected in comparison of AlN: Er and AlN: ErYb. A magnetic field of 1000 G was applied to AlN: ErYb resulting in an increase in intensity of the major peak at 561nm with a splitting, creating a secondary peak at 564.5 nm. Biomedical applications can be used from the high penetration ability of lower wavelength lasers and the use of a magnetic field, which is not harmful to the human body. Enhanced green emission in erbium can be useful in future optical, photonic, and electrical devices. / Department of Physics and Astronomy

In this thesis, I have developed a tunable two-color two-stage ultrafast Yb:fiber chirped pulse amplifier for the generation of short-pulse mid-infrared (MIR) radiation in the long-wavelength side of the "molecular fingerprint" (2.5-25 μm) using difference frequency generation (DFG) technique. The two colors called blue and red are in the wavelengths 1.03-1.11 μm and are amplified simultaneously in the same Yb-doped fiber amplifier (YDFA) stages in order to reduce the induced environmental noise on the phase difference of the pulses and to minimize the complexity and system cost. I will present numerical simulations on the two-stage YDFA system to amplify a two-color spectrum in the wavelengths 1.03-1.11 μm. The first and second YDFA called preamplifier and main amplifier are single-clad, single-mode and double-clad, single-mode YDFA respectively. From numerical simulations, the optimal length of the preamplifier to have equal power at two colors centered at 1043 nm and 1105 nm are in agreement with experimental results. It is well known that the power of MIR radiation generated by difference frequency mixing of two wavelengths scales up with the product of mixing powers in a fixed-field approximation. Furthermore, for the gain narrowing effect on the short-wavelength side of the YDFA gain profile, the spectral bandwidth of the blue color decreases resulting in pulse broadening. In addition, for the two colors separated largely, the amplified spontaneous emission is intensified. Considering the cited factors, I will present the modeling results on the two-color, two-stage YDFA system that the product of the power of the two colors is maximized for a maximized wavelength separation between the two mixing colors and a minimized gain narrowing on the blue color in order to build an as broadly tunable and powerful as possible ultrafast mid-infrared source by difference frequency mixing of the two colors. In this research, I achieved a wavelength separation as broad as 71 nm between pulses centered at 1038 nm and 1109 nm from the two-color ultrafast YDFA system. I achieved combined average powers of 2.7 W just after the main amplifier and 1.5 W after compressing the two-color pulses centered at 1041 nm and 1103 nm to nearly Fourier transform limited pulses. From autocorrelation measurements, the full width at half maximum (FWHM) of the compressed two-color pulses with the peak wavelengths of 1041 nm and 1103 nm was ~500 fs. By mixing the tunable two-color pulses in a 1-mm-thick GaSe crystal using DFG technique, I achieved tunable short-pulse MIR radiation. In this research, I achieved short-pulse MIR radiation tunable in the wavelengths 16-20 μm. The MIR tuning range from the lower side was limited to the 16 μm because of the 71-nm limitation on the two-color separation and from the upper side was limited to the 20 μm because of the 20-μm cutoff absorption wavelength of GaSe. Based on measured MIR spectra, the MIR pulses have a picosecond pulse duration in the wavelengths 16-20 μm. The FWHM of measured spectra of the MIR pulses increases from 0.3 μm to 0.8 μm as the MIR wavelength increases from 16 μm to 20 μm. According to Fourier transform theory, the FWHM of the MIR spectra corresponds to the bandwidth of picosecond MIR pulses assuming that the MIR pulses are perfectly Fourier-transform-limited Gaussian pulses. In this research, I achieved a maximum average power of 1.5 mW on short-pulse MIR radiation at the wavelength 18.5 μm corresponding to the difference frequency of the 500-fs two-color pulses with the peak wavelengths of 1041 nm and 1103 nm and average powers of 1350 mW and 80 mW respectively. Considering the gain bandwidth, Ti:sapphire is a main competitor to the YDFA to be used in the two-color ultrafast laser systems. In the past, the broad gain bandwidth of Ti:sapphire crystal has resulted in synchronized two-color pulses with a wavelength separation up to 120 nm. Apart from its bulkiness and high cost, Ti:sapphire laser system is limited to a watt-level output average power at room temperature mainly due to Kerr lensing problem that occurs at high pumping powers. In comparison, YDFA as a laser amplifier has a narrower gain bandwidth but it is superior in terms of average power. Optical parametric generation (OPG) and optical parametric amplification (OPA) techniques are two competitors to DFG technique for the generation of short-pulse long-wavelength MIR radiation. Although OPG offers a tunability range as broad as DFG, the MIR output power is lower because of the absence of input signal pulses. From the OPA technique, the tunability range is not as broad as the DFG technique due to limitations with the spectral bandwidth of the optical elements. Currently, quantum cascade lasers (QCLs) are the state-of-art MIR laser sources. At the present time, the tunability range of a single MIR QCL is not as abroad as that achieved from the DFG technique. More, mode-locked MIR QCLs are not abundant mainly because of the fast gain recovery time. Thus, the generation of widely tunable short-pulse MIR radiation from DFG technique such as that developed in this thesis remains as a persistent technological solution. The application of the system developed in this thesis is twofold: on one hand, the tunable two-color ultrashort pulses will find applications for example in pump-probe ultrafast spectroscopy, short-pulse MIR generation, and optical frequency combs generation. On the other hand, the short-pulse MIR radiation will find applications for example in time-resolved MIR spectroscopy to study dynamical behavior of large molecules such as organic and biological molecules.