We report a review on our recent developments in Yttebium and Neodymium doped laser ceramics, along two main research lines. The first is the design and development of Yb:YAG ceramics with non uniform doping distribution, for the management of thermo-mechanical stresses and for the mitigation of ASE: layered structures have been produced by solid state reactive sintering, using different forming processes (spray drying and cold press of the homogenized powders, tape cast of the slurry); samples have been characterized and compared to FEM analysis. The second is the investigation of Lutetium based ceramics (such as mixed garnets LuYAG and Lu2O3); this interest is mainly motivated by the favorable thermal properties of these hosts under high doping. We recently obtained for the first time high efficiency laser emission from Yb doped LuYAG ceramics. The investigation on sesquioxides has been focused on Nddoped Lu2O3 ceramics, fabricated with the Spark Plasma Sintering method (SPS). We recently achieved the first laser emission above 1 W from Nd doped Lu2O3 ceramics fabricated by SPS.
The ytterbium-doped crystals emitting around 1 μm under laser-diode pumping between 900-980 nm have received an
increasing interest in recent years as solid-state laser materials for high power or ultra-fast lasers. In this paper, our main
objective is to contribute to Yb3+-doped fluorides mainly on CaF2 cubic host which are characterized by a high value of
the thermal conductivity (9.5 W m-1 K-1) as high as YAG. Yb3+-doped CaF2, mono-doped and concentration gradient
fibres were grown by both, the laser heated pedestal growth (LHPG) method and by the Czochralski method. Concerning
Yb3+ excited state dynamics, the concentration dependence of the 2F5/2 decay time shows a competition between self-trapping
and self-quenching processes. Main parameters useful for a theoretical approach of laser potentiality will be
given and laser emission under InGaAs laser-diode pumping will be shown.
We investigated the CW free-running and repetitive modulation in the kHz frequency domain of a passively Q-switched, diode-pumped Yb:YAG, Yb:GGG and Yb:KYW lasers, by using Cr4+:YAG as a saturable absorber. The results presented here are focused towards the design of a passively Q-switched Yb doped garnets or Yb doped tungstates microlaser. The free-running performance of Yb:YAG, Yb:GGG, Yb:KGW and Yb:KYW were characterized, and experimental parameters such as gain and loss were evaluated. We carried out a fit between our experimental results and an existing numerical model, which relates the experimental and the physical parameters of the ytterbium diode-pumped system to the minimal threshold pumping power. The best performance among the laser crystals was obtained for Yb:YAG laser. A maximum peak power of ≈4.5-kW, at an average output power of 1.32-W, were extracted with of ≈25 % extraction efficiency.
Electron paramagnetic resonance (EPR) measurements of CaF2:Yb (5 mol. %) single crystals were performed for lattice sites substituted by Yb ions and also for the possibility of Yb3+ pairs arising. Among eight lines observed in the EPR spectrum, with g = 4.293, 4.1, 3.965, 3.665, 3.433, 3.13, 3.054, 2.894 we think mainly the lines coming from different isotopes of Yb3+ isolated ions of cubic symmetry one can distinguish: 170Yb3+ I=0, 171Yb3+ I=1/2 and 173Yb3+ I=5/2, but one can not exclude the lines coming from Yb3+ pairs. All of the lines have got an axial symmetry along the crystallographic axis, since the lines do not move with angular variation in the planes parallel and perpendicular to the axis. One can observe also the extra line in magnetic field orientation in every plane at 45°, with the B0≈191 mT. The unidentified line corresponds to non-axial Yb3+ center or unknown impurity. The components of A and g tensors of the spin Hamiltonian for cubic symmetry were calculated. Temperature dependence of EPR lines shows agreement with the Curie law for most of the lines. Peak-to-peak linewidth changes continuously within 20 mT range for "as-grown" crystals, while shows distinct increase above 25 K for γ-irradiated ones. It suggests strong ferromagnetic coupling between neighbours Yb3+ and Yb2+ ions the latter being created due to Compton electron capture. So, Yb3+ co-exists with Yb2+ after the Yb3+-Yb2+ conversion under influence of γ-irradiation and/or annealing in hydrogen. It seems the Yb2+ centers arising in CaF2:Yb (5 mol. %) single crystal after γ-irradiation are related to Yb3+, as an effect of recharging one of Yb3+ ion from a pair. Absorption measurements of CaF2 highly doped with Yb3+ (0.5 mol. %, 5 mol. % and 30 mol. %) reveal the shifting of the IR maxima of 921 and 980 nm characteristic for 0.5 mol. % doping of Yb3+ towards the centrum of IR band (927 and 976 for 30 mol. % of Yb3+). Raman spectrum shows localized phonon centered at about 64 cm-1 being confirmation of the Yb3+ pairs presence in the 5 mol. % of Yb3+ doped CaF2 crystal.
Diode pumping of a laser-stress-free, Nd( 5 % at.):KGW, grown by top nucleated floating crystal (TNFC) method, is presented. The diode-pumped laser was operated both in the free-running and passively Q-switched operating modes. Under optimized conditions of resonator and optics, the Nd:KGW disk (1.3 mm in thickness), produced at room temperature an efficient free-running, TEM00 output with maximum power of 0.4-W, with 75 % slope efficiency and 51 % total laser efficiency. Under slightly different experimental conditions the laser was passively Q-switched by using Cr4+:YAG as saturable absorber. The passively Q-switched laser produced modulated pulses at average frequencies in the range of 10-20 kHz, with pulsewidth of ≈180 nsec, with an average output power obtained was 30 mW at the maximumpumping power level. The results presented here indicate the potential Nd:KGW crystals grown by TNFC growth method, as candidates for concentrated, stress free diode pumped microlasers in a large variety of wavelengths, including the eye-safe range.
Diode pumping of a stress-free, Nd(5%at.):KGd(WO4)2, grown by top nucleated floating crystal (TNFC) method, is presented. The diode-pumped laser was operated both in the free-running and passively Q-switched operating modes. Under optimized conditions of resonator and optics, the disk (1.3 mm in thickness), produced at room temperature an efficient free-running, TEM00 output with maximum power of 0.4 W, with 75% slope efficiency and 51% total laser efficiency. The results presented here indicate the potential Nd:KGd(WO4)2 crystals grown by TNFC growth method, as candidates for concentrated, stress free diode pumped microlasers in a large variety of wavelengths, including the eye-safe range.
New and original monocrystalline samples having a continuous longitudinal concentration gradient are used to study dynamical processes of resonant transitions in rare earth doped laser crystals like Y2O3 sesquioxide and YAG garnet. This fast and simple method allows to measure the radiative lifetime, the influence of radiation trapping, impurity quenching and RE pairs or clusters on the excited-state lifetime as a functon of the dopant concentration. Examples in Yb3+, Er3+ and Ho3+ rare earth ions are presented.
The renewal of second order non-linear crystals is very strong in laser materials optics. We are involved in the search of new systems based upon highly non-linear niobate crystal family. Among these crystals, Ba2NaNb5O15 (BNN) and K3Li2-xNb5+xO15+2x (KLN, 0.15 < x < 0.5) with a tungsten bronze-type structure are very efficient materials for the obtention of respectively green and blue laser light by frequency doubling or by self-frequency doubling after doping by Nd3+ ions. Unfortunately, BNN and KLN are difficult to grow by conventional techniques such as Czochralski without cracks caused by a strong lattice change occurring during cooling of the crystals. In addition, microtwins in BNN crystals and compositional inhomogeneities in KLN ones are often encountered. The obtention of good quality and crackless BNN and KLN single crystals doped with different amounts of Nd2O3 is reported. The crystals were grown by the laser heated pedestal growth technique. This method allowed to obtain good quality and homogeneous crystals of BNN and KLN overcoming the problems encountered with other growth techniques. More particularly, for BNN crystals, a structural transition between orthohombic and tetragonal symmetry was found to occur for a Nd3+ amount between 2 and 3 atomic percent avoiding the microtwinning which disturbs the optical properties of the crystals. Low temperature spectroscopy revealed that Nd3+ ions substitute both Ba2+ and Na+ ions in the pentagonal and square sites of the tungsten bronze-type structure of BNN whereas they substitute only K+ ions in the pentagonal sites of that of KLN. Non- critical phase matching at room temperature was also investigated for both materials.
The mutual static crystal field perturbations produced by near sensitizer and activator ions shift the energy levels and modify the radiative and energy transfer characteristics. The selective and discrete nature of these effects transforms the ensembles of sensitizer and activator ions into inhomogeneous systems and modify the spectral and temporal characteristics of emission from activator ions in sensitized laser crystals. These effects are exemplified for Cr3+ or Fe3+ sensitized emission of Tm3+:YAG.
The spectroscopic properties of F3+ ions in tetrahedral sites in garnets, together with the good packing of these sites around the dodecahedral position occupied by rare-earth ions, favor a very efficient energy transfer from Fe3+ to TM3+. Since Fe3+ does not introduce additional losses, this ion is a potential sensitizer for Tm3+ laser emission.
Spectroscopic studies using laser induced fluorescence and numerical modelling of energy transfer and back transfer mechanism are reported in Er:Tm:Ho:YLF, Cr:Tm:Ho:YAG and Cr:Tm:YAG laser crystals at various temperatures (10 K - 300 K). Direct energy transfer from Tm3+ excited states to Ho3+5I7 emitting level was observed and analyzed both in YAG and YLF. Further analysis of Cr3+ and Tm3+ time-dependent emission curves indicate a strong correlation of chromium- thulium pairs. Pulsed operation of holmium laser at high temperature will be presented.
The standard expression for the excited state acceptor concentration in codoped solid-state materials is modified to include the possibility of non-radiative acceptor de-excitation. The chromium and thulium time-dependent emission in yttrium aluminum garnet (YAG) is then studied; evidence is given for the identification of the tendency for localized correlated chromium-thulium pairs in the crystalline material.
The possibility of sensitization of rare-earth laser active ions with infrared (especially two- micron) emission by Fe3+ is discussed. The spectroscopic and luminescence decay measurements on Fe, Tm or Fe:Tm doped GGG or YAG show that a very efficiency energy transfer from Fe3+ in tetrahedral sites to Tm3+ takes place showing prospects for new sensitization schemes.
Work being done on solid-state lasers in a single laboratory is reviewed. Recent results on broadly tunable laser systems based on transition metal ions are addressed, discussing excited-state absorption measurements and the search for new emitting centers. The main emission spectra obtained with the rare earth doped laser materials Nd(3+), Er(3+), Tm(3+), and Ho(3+) are shown and discussed.
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