Laser operation of the new stoichiometric crystal KYb(WO4)2

We demonstrate for the first time laser operation with the monoclinic stoichiometric crystal KYb(WO₄)₂ (hereafter KYbW). Lasing on the ² F _5/2 ?² F _7/2 transition of Yb³⁺ at room temperature has been achieved near 1074 nm with >41% slope efficiency (>26% maximum conversion efficiency) using a 0.5-mm-thick plate of KYbW. This new laser material holds great promise for diode-pumped high-power lasers, thin-disk and waveguide designs as well as for ultrashort (ps/fs) pulse laser systems. Received: 10 October 2001 / Revised version: 19 November 2001 / Published online: 17 January 2002     

Laser-related spectroscopy of ion-doped crystals for tunable solid-state lasers

In this work an overview of transition metal (TM) ion- and rare earth (RE) ion-doped crystals for application as tunable solid-state lasers will be given. Spectroscopic and laser results will be presented including recent research and advances in this field. Within this work tunability is defined as the possibility to achieve laser oscillation in the vibronic sideband of a transition. Tunable solid-state lasers are of interest for a wide field of applications, e.g. in scientific research, in medicine, for measurement and testing techniques, ultra short pulse generation, and communication. They can also be used as coherent light sources for second-harmonic generation, for optical parametric oscillators, and for sum- and difference-frequency generation. Tunable laser media based on 3d?3d transitions of transition-metal ions and 4f?5d transitions of rare-earth ions cover nowadays almost the whole spectral range between 270 nm and 4500 nm, see Fig. 1 [1-15]. In comparison to laser systems based on the 4f?4f transitions of trivalent rare-earth ions, tunable lasers based on 3d?3d and 4f?5d transitions are in general affected by a higher probability of excited-state absorption (ESA), a higher probability of non-radiative decay, and a higher saturation intensity leading to higher laser thresholds. Often laser oscillation cannot be obtained at all. These general topics will be considered in Sect. 1, where the basic aspects of tunable solid-state lasers are discussed: these are the preparational, the spectroscopic, and the laser aspect. In Sect. 2, the investigation of transition metal ion-doped crystals with respect to the realization of tunable laser oscillation is presented. The work is focused on transition-metal ions of the 3d row (Fe row) and divided into two subsections according to the octahedral and tetrahedral coordinations of the ion investigated. Each subsection is structured according to the electron configurations: 3d¹, 3d³, 3d⁴, and 3d⁸ for the octahedrally coordinated ions and 3d¹, 3d², and 3d⁴ for the tetrahedrally coordinated ions. Section 3 deals with interconfigurational transitions of divalent and trivalent rare-earth ions. Finally, in Sect. 4 the work is summarized. Received: 22 December 2000 / Published online: 30 March 2001     

Green up-conversion of Er3+ in KGd(WO4)2 crystals. Effects of sample orientation and erbium concentration

Pumping with infrared light resonant to the energy position of ⁴ I _11/2 and ⁴ I _9/2 multiplets respectively has excited green up-conversion of Er³⁺ in KGd(WO₄)₂ single crystal. At room temperature the maximum green-emission intensity is achieved by pumping with light polarized parallel to the C₂ symmetry axis of the crystal (//p) at 981 and 801.5 nm, while pumping with light parallel to the principal m axis (//m) has maximum up-conversion at 978.2, 806 and 800 nm. The emission is weakly polarized. The maximum of the emission peaks at 547.8 nm if the light is analyzed parallel to the C₂ axis or at 552.4 nm for light perpendicular to it. The largest emission intensity was achieved with an erbium concentration about 3×10²⁰ cm^-3. A schematic model of the up-conversion process is suggested. Received: 4 July 2000 / Published online: 22 November 2000     

Relaxation dynamics of excited states of Tm3+ in SrGdGa3O7 crystals activated with Tm3+ and Tb3+

3 H₄ and ³F₄ states of Tm in SrGdGa₃O₇ single crystal was evaluated. Tm-Tb energy transfer reduces effectively the lifetime of terminal level in a potential ³H₄-³F₄ laser transition but gives rise to parasitic nonradiative relaxation of the initial ³H₄ level. SrGdGa₃O₇ crystal single doped with thulium possesses combination of properties advantageous for laser oscillations near 1.9 μm, namely high rate of cross relaxation process leading to population buildup on the initial ³F₄ level and relatively high crystal field splitting of the ground ³H₆ level. Received: 25 April 1996/Revised version: 10 October 1996     

Infrared excited-state absorption and stimulated-emission cross sections of Er3+-doped crystals

Detailed spectra of the excited-state absorption and the stimulated-emission cross-sections of Er³⁺ -doped Y₃Al₅O₁₂, YAlO₃, LiYF₄, and KYF₄ crystals are analyzed in the infrared wavelength regions from 700 to 2100 nm. The spectra were measured with a pump and probe technique employing a double modulation scheme. For Er (2%): Y₃Al₅O₁₂ also the stimulated emission at 3 µm and the reabsorption due to excited-state absorption from the lower laser level are investigated.     

Optical spectra and luminescence dynamics of Pr3+ and Nd3+ in SrLaAlO4 single crystals

Single crystals of SrLaAlO₄: Pr³⁺ and SrLaAlO₄: Nd³⁺ have been grown by the Czochralski method and their optical properties have been studied for different activator concentrations. The absorption and emission spectra of the activators are inhomogeneously broadened because the Sr²⁺ and La³⁺ ions are distributed randomly on the sites ofC ₄ symmetry, however, the symmetry selection rules are still obeyed. Strong self-quenching of the praseodymium luminescence occurs by cross relaxation which is supposed to be assisted by phonon emission in the case of the³ P ₀ level. Self-quenching of Nd³⁺ luminescence disappears at low temperature indicating that the condition of resonance in the cross-relaxation process is fulfilled only for higher components of the ground state.Institute of Low Temperature and Structure Research, Polish Academy of Sciences, Wroclaw, Poland     

Efficient laser operation and continuous-wave diode pumping of Cr2+:ZnSe single crystals

Efficient continuous-wave laser operation of Cr²⁺:ZnSe was demonstrated with an output power of 1400 mW at an absorbed pump power of 1900 mW from a Tm:YAG laser. Under continuous-wave diode pumping at 1.54 μm an output power of 15 mW was obtained from a Cr⁺²:ZnSe laser. Excited state absorption is shown to be negligible in the pump and laser spectral region. Received: 12 October 2000 / Published online: 30 November 2000     

Self-starting five optical cycle pulse generation in Cr<Superscript>4+</Superscript>:YAG laser

We report stable self-starting near-transform-limited 26-fs pulses at 250-mW output power from a Kerr-lens mode-locked (KLM) Cr⁴⁺:YAG laser using chirped mirrors in combination with prisms. The highest output power achieved in KLM regime was 600 mW at 55-fs pulse duration. The experimental results agree well with the results of theoretical analysis with respect to KLM self-starting ability and stability against continuous-wave and multi-pulse operation. Parameter ranges for stable transform-limited KLM pulses as well as the shortest achievable pulse durations are established. Using an InGaAs-InP semiconductor saturable absorber mirror we could obtain self-starting 57-fs pulses at the average output power of 200 mW. Two-photon absorption was found to be the main mechanism favoring the multiple-pulse operation. Received: 2 May 2002 / Revised version: 16 July 2002 / Published online: 8 January 2003 RID="*" ID="*"Corresponding author. Fax: +43-1/58801-38799, E-mail: sorokina@tuwien.ac.at     

Spectroscopic characterisation of LaGaO3:Er3+ crystals

LaGaO₃ crystals doped with Er³⁺ ions were grown by the Czochralski method and their optical properties were examined. The Er³⁺ energy levels have been determined from the low-temperature absorption and emission spectra. The results of Judd–Ofelt analysis are presented and compared with experimental data. The emission cross sections are determined for the ⁴ I _13/2→⁴ I _15/2 (1.55 μm) and ⁴ I _11/2→⁴ I _13/2 (2.85 μm) transitions of erbium. Received: 6 December 1999 / Revised version: 10 February 2000 / Published online: 27 April 2000     

Spectroscopic characterization of a Tm3+:SrGdGa3O7 crystal

3 O₇ crystal have been recorded at room temperature and at approximately 8 K. Room-temperature luminescence lifetimes of ¹D₂, ¹G₄, ³H₄, and ³F₄ states have been measured for Tm concentration ranging from [%at.]0.5 to [%at.]9. Based upon these data the crystal field splitting of luminescent states has been derived and radiative transitions rates have been evaluated. Strong self-quenching of luminescence originating in the ¹G₄ and ³H₄ states has been found in this activator–host combination. Peak emission cross section of the potential laser transition at 1800 nm was determined to be 3.9×10^-21 cm² and the gain coefficient versus wavelength was estimated and discussed. Received: 14 April 1998/Revised version: 10 August 1998     

New green self-frequency-doubling diode-pumped Nd:Ca4GdO(BO3)3 laser

3+ :Ca₄GdO(BO₃)₃ (Nd:GdCOB). 21 mW of green cw laser emission for an absorbed pump power of 820 mW were achieved under laser diode-pumping. 64 mW of green cw laser output were obtained with 1 W of absorbed pump power under titanium-sapphire pumping. Its availability in large-size crystals with good optical quality makes Nd:GdCOB a true challenger to the best SFD laser crystal reported so far: Nd:YAl₃(BO₃)₄ (Nd:YAB or NYAB). Received: 2 March 1998/Revised version: 20 May 1998     

Spectroscopic properties and exicted-state relaxation dynamics of Er3+ in LiNbO3

Nonequivalent Er³⁺ sites in LiNbO₃ crystals have been evidenced by low-temperature optical absorption measurements. The radiative transition rates for the ⁴ S _3/2, ⁴ F _9/2, ⁴ I _9/2, ⁴ I _11/2, and ⁴ I _13/2 levels have been evaluated by the Judd-Ofelt method, and the contribution of multiphonon relaxation to the decay of excited states has been estimated. The quantum efficiency of the ⁴ I _11/2 level has been estimated to be 6% only, thus the excitation of levels lower than ⁴ S _3/2 is expected to populate efficiently the ⁴ I _13/2 level.     

Continuous-wave tunable Cr2+:ZnS laser

We report the first continuous-wave tunable over ∼280 nm around 2.3 μm room-temperature operation of a chemical vapor transport-grown and diffusion-doped Cr²⁺:ZnS laser, pumped by a Co:MgF₂ laser at 1.67 μm and generating over 100 mW of output power at 16% slope efficiency. The self-consistent results of the laser and spectroscopic analysis demonstrate a large potential of this crystal as an active medium for diode-pumped tunable mid-infrared sources. Received: 7 January 2002 / Revised: 14 March 2002 / Published online: 2 May 2002     

Comparative investigation of spectroscopic and laser emission characteristics under direct 885-nm pump of concentrated Nd:YAG ceramics and crystals

A high-resolution spectroscopic and emission-decay investigation of highly concentrated Nd:YAG single crystals and ceramics shows that the state of the Nd³⁺ ions and their interaction in these materials are similar and can be used for construction of efficient solid-state lasers directly pumped in the emitting level. This possibility is demonstrated by continuous-wave emission of concentrated Nd:YAG crystals with up to 3.5 at. % Nd and ceramics with up to 6.8 at. % Nd under resonant 885-nm end pump. Received: 28 May 2001 / Final version: 17 August 2001 / Published online: 10 October 2001     

Dynamics of the Yb3+ to Er3+ energy transfer in LiNbO3

The energy transfer dynamics between Yb³⁺ and Er³⁺ ions in lithium niobate is investigated after ytterbium-pulsed excitation at 920 nm. The sensitisation of the LiNbO₃:Er³⁺ system with Yb³⁺ ions does not modify the lifetime of the ⁴I_13/2 erbium level (1.5-μm emission), whereas it induces a marked, concentration-dependent change in the lifetime of the ²F_5/2 (Yb³⁺) and ⁴S_3/2 (Er³⁺) multiplets (1060-nm and 550-nm emissions, respectively). The results are analysed by using the rate-equation formalism and cross-relaxation model for the energy transfer. Received: 15 October 1998 / Revised version: 24 November 1998 / Published online: 24 February 1999     

New materials for optical cooling

Well-characterized solid-state laser materials are evaluated for performance in optical refrigeration as well as radiation-balanced laser systems. New figures-of-merit are developed and applied to ytterbium-doped materials. Superior performance is predicted for high-cross-section tungstate materials. Photothermal deflection experiments on samples of Yb³⁺-doped KGd(WO₄)₂ confirm anti-Stokes fluorescence cooling. This is the first observation of optical cooling in a crystal. Received: 1 February 2000 / Revised version: 15 June 2000 / Published online: 13 September 2000     

Spectroscopic analysis and laser parameters of Nd3+ in Ca3Sc2Ge3O12 garnet crystals

3 Sc₂Ge₃O₁₂ (CaSGG) single crystals with the garnet structure have been grown by means of the flux growth technique. The doping with Nd³⁺ and Mg²⁺ (as charge compensator) yields samples suitable for optical spectroscopy experiments. The absorption and emission properties have been measured at temperatures ranging from 10 to 298 K. The emission spectra give evidence of the presence of non-equivalent Nd³⁺ sites. The decay time of the 1.06-μm emission band has been measured as a function of temperature and incident power. The intensities of the 298 K absorption transitions have been analyzed by means of the Judd–Ofelt theory. The radiative lifetimes, the branching ratios (β), and the spontaneous emission probabilities have been evaluated for the ⁴F_3/2 excited state using the calculated intensity parameters. The stimulated-emission cross sections and the branching ratios have been estimated from the experimental data for the most important laser transitions indicating that this crystal can be considered an interesting material for solid-state laser applications. Received: 2 June 1998 / Revised version: 28 October 1998 / Published online: 24 February 1999     

Structural and optical characterization of Er3+/Yb3+-doped LiNbO3

We report the dependence of the unit-cell parameters and the extraordinary and ordinary refractive indices of Er³⁺/Yb³⁺-codoped LiNbO₃ crystals. Both properties depend in a non-monotonic manner on the Er³⁺/Yb³⁺ content. A singularity was observed at concentrations of 1.1-1.2 mol. % in the crystal (0.6-0.7 mol. % in the melt). In the same way the Er and Yb concentration influences the periodically poled lithium niobate formation. The observed behavior of refractive indices and unit-cell parameters of Er³⁺/Yb³⁺-codoped LiNbO₃ crystals could be explained in terms of the RE³⁺-ion concentration affecting the Li-vacancy concentration and the RE³⁺-ion positions in the crystal. Received: 21 May 2001 / Revised version: 22 August 2001 / Published online: 23 October 2001     

Efficient and highly photostable solid-state dye lasers based on modified dipyrromethene.BF2 complexes incorporated into solid matrices of poly(methyl methacrylate)

We report on the laser action of modified dipyrromethene.BF₂ complexes both dissolved in poly(methyl methacrylate) and copolymerized with methyl methacrylate. All recently synthesized dyes have the chromophore core of laser dye pyrromethene 567, differing in the substituent in position 8. The new dyes showed important and most significant increases in both lasing efficiency and photostability. When the laser samples were pumped transversely at 534 nm, laser emission was obtained with efficiencies of over 30% in most cases, to be compared with a lasing efficiency of 12% exhibited by reference dye pyrromethene 567 under the same experimental conditions. Some of the materials exhibited highly photostable laser action, with no sign of degradation in the laser output after 60000 pump pulses at the same position of the sample at a repetition rate of 10 Hz, whereas the laser emission of reference dye pyrromethene 567 dropped to zero after less than 40000 pump pulses. Received: 19 November 2002 / Revised version: 20 February 2003 / Published online: 9 April 2003 RID="*" ID="*"Corresponding author. Fax: +34-91/564-2431, E-mail: acostela@iqfr.csic.es     

Passive Q-switching at 1.54 μm of an Er–Yb: GdCa4O(BO3)3 laser with a Co2+: MgAl2O4 saturable absorber

We report, for the first time to our knowledge, efficient passive Q-switching of the 1.54-μm laser transition in an Er–Yb-doped crystalline medium. The laser configuration is a compact microchip design that is suitable for a range of practical applications such as range finding and lidar. The slope efficiency of 11.6%, pulse duration of 5–6 ns and average output power of 88 mW are all comparable with standard Er–Yb:glass lasers.