The optical properties of Yb3+ ions in LiTaO3:Nd,Yb crystals

3+ ions excited by energy transfer from Nd³⁺ ions in LiTaO₃:Nd, Yb crystals are presented. The emission band of Yb³⁺ ions is broad, due to the strong phonon-coupling and to the relative large Stark-splitting of the ground ²F_7/2 multiplet. The emission cross-section was evaluated by the reciprocity method, and a value of 0.53×10^-20 cm² was obtained. The gain coefficients derived for the inversion parameters in the range 0.05 to 0.5 indicate positive gain in the 985–1070 nm range. Received: 17 March 1997/Revised version: 10 June 1997     

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     

Material tensor parameters of LiNbO3 relevant for electro- and elasto-optics

The complete set of self-consistent parameters of nominally undoped LiNbO₃ crystals of congruent composition that describe the electro-optic, piezoelectric, elasto-optic, elastic, and dielectric response has been determined by numerically evaluating available measurements. The parameters were determined at room temperature and consist of the low-frequency clamped dielectric constants ε^S _ij, elastic stiffness constants at constant electric field C^E _ijkl, piezoelectric stress coefficients e_ijk, elasto-optic constants at constant electric field p^E _ijkl, and clamped electro-optic coefficients r^S _ijk. It is shown that the complete set is required for calculating the effective electro-optic coefficients and dielectric constants in photorefractive applications of LiNbO₃. Received: 4 January 2002 / Revised version: 1 February 2002 / Published online: 14 March 2002     

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     

Visible and infrared dispersion of the refractive indices in periodically poled and single domain Nd:Mg:LiNbO3 crystals

3 crystals are measured in the transparency region (with the accuracy ±0.0002) and for the upper phonon polariton branch (with the accuracy ±0.003–±0.05), from 0.44 μm up to 10.5 μm. The method of spontaneous parametric light scattering is used for measurement of the ordinary refractive index dispersion in the mid-infrared region and for determination of the domain grating period d=5.6±0.2 μm in the periodically-poled crystal. Received: 29 January 1997/Revised version: 10 July 1997     

Site-selective spectroscopy of Er3+:Ti:LiNbO3 waveguides

Starting from previous investigations in LiNbO₃ bulk crystals, we studied the optical properties of Er³⁺ ions in Ti:LiNbO₃ channel waveguides and investigated the waveguide-specific lattice environment of the Er³⁺ ions (“sites”) caused by the doping method used and the presence of a large number of Ti⁴⁺ ions. For that purpose the method of combined excitation–emission spectroscopy was applied for the first time to waveguides at low temperatures. Comparing the spectroscopic results obtained for the green, red, and near-IR luminescence (λ≈550, ≈650 and ≈980 nm) under direct (450 nm), 2-step (980 nm), and 3-step (1.5 μm) laser excitation, we found several distinguishable Er³⁺ sites which in terms of energy levels and relative numbers are similar to those in bulk material, but exhibit significantly different up-conversion efficiencies and strongly inhomogeneously broadened transitions. Moreover, we were able to distinguish isolated and cluster Er³⁺ sites by their characteristic excitation and emission transition energies and studied the respective excitation/relaxation channels. The cluster sites are most efficient in the up-conversion process, especially under 3-step excitation. Using accepted microscopic models for Er³⁺ and Ti⁴⁺ incorporation into the LiNbO₃ crystal lattice, the site distribution and up-conversion mechanisms are elucidated and their consequences for laser applications in different spectral regions are discussed. Received: 16 November 2000 / Published online: 21 March 2001     

Crystalline structure and optical spectroscopy of Er3+-doped KGd(WO4)2 single crystals

4 )₂ single crystals doped with Er³⁺ have been grown by the flux top-seeded-solution growth method. The crystallographic structure of the lattice has been refined, being the lattice constants a=10.652(4), b=10.374(6), c=7.582(2) Å, β=130.80(2)°. The refractive index dispersion of the host has been measured in the 350–1500 nm range. The optical absorption and photoluminescence properties of Er³⁺ have been characterised in the 5–300 K temperature range. At 5 K, the absorption and emission bands show the (2J+1)/2 multiplet splittings expected for the C₂ symmetry site of Er in the Gd site. The energy positions and halfwidths of the 72 sublevels observed have been tabulated as well as the cross sections of the different multiplets. Six emission band sets have been observed under excitation of the ⁴F_7/2 multiplet. The Judd–Ofelt (JO) parameters of Er³⁺ in KGW have been calculated: Ω₂=8.90×10^-20 cm², Ω₄=0.96×10^-20 cm², Ω₆=0.82×10^-20 cm². Lifetimes of the ⁴S_3/2, ⁴F_9/2, and ⁴I_11/2 multiplets have been measured in the 5–300 K range of temperature and compared with those calculated from the JO theory. A reduction of the ⁴S_3/2 and ⁴I_11/2 measured lifetimes with increasing erbium concentration has been observed, moreover the presence of multiphonon non-radiative processes is inferred from the temperature dependence of the lifetimes. Received: 15 December 1997/Revised version: 10 July 1998     

Spectral line broadening mechanism of Er3+ transitions in Er:Ti:LiNbO3 channel waveguides

In order to elucidate the interaction effects among the various defects present in a LiNbO₃-based integrated optical device, we investigated the change of the optical properties of Er³⁺ ions under the application of an external electric field and hydrostatic pressure. We obtained for stoichiometric bulk material a complete picture of the field-induced spectral shifts as a function of transition and site. As a first important application of these results we were able to clarify the mechanism of spectral broadening of the Er³⁺ transitions in Ti:Er:LiNbO₃ channel waveguides. By selecting different waveguide modes for excitation and using highly selective double-resonance excitation with two lasers, we found that the [Ti⁴⁺] concentration gradient caused by the indiffusion results in an internal E-field gradient. This translates, due to the averaging within the guided mode, into mode-dependent spectral line broadening. Received: 24 May 2001 / Published online: 23 October 2001     

Structural and optical properties of thermal evaporated magnesium phthalocyanine (MgPc) thin films

X-ray powder diffraction (XRD) of MgPc indicated that the material in the powder form is polycrystalline with monoclinic structure. Miller indices, h k l, values for each diffraction peak in XRD spectrum were calculated. Thermal evaporation technique was used to deposit MgPc thin films. The XRD studies were carried out for MgPc thin films where the results confirm the amorphous nature for the as-deposited films. While, polycrystalline films orientated preferentially to (1 0 0) plane with an amorphous background were obtained for films annealed at 623 K for 3 h. Optical properties of MgPc thin films were characterised by using spectrophotometric measurements of transmittance and reflectance in the spectral range from 190 to 2500 nm. The refractive index, n, and the absorption index, k, were calculated. According to the analysis of dispersion curves, the parameters, namely; the optical absorption coefficient (α), molar extinction coefficient (?_molar), oscillator energy (E_os), oscillator strength (f), and electric dipole strength (q²) were also evaluated. The recorded absorption measurements in the UV-vis region show two well defined absorption bands of phthalocyanine molecule; namely the Q-band and the Soret (B-band). The Q-band showed its splitting characteristic (Davydov splitting), and ΔQ was obtained as 0.15 eV. The analysis of the spectral behaviour of the absorption coefficient (α), in the absorption region revealed indirect transitions. The transport and the near onset energy gaps were estimated as respectively 2.74 ± 0.02 and 1.34 ± 0.01 eV.     

Optical characterization of Cr3+ centers in LiNbO3

Low-temperature luminescence spectra of stoichiometric Cr:LiNbO₃, congruent Cr:LiNbO₃ and congruent Cr,Mg:LiNbO₃ were studied. Dominant low-field and minor high-crystal-field optical centers are the Cr³⁺ impurity ions that preferentially occupy Li⁺ sites (Cr_Li) in the Cr:LiNbO₃ crystals. Low-field centers related to Cr³⁺ substitution of Nb⁵⁺ (Cr_Nb) occur in addition to Cr_Li in co-doped Cr,Mg:LiNbO₃ samples. Application of high hydrostatic pressure leads to the transformation of dominant Cr³⁺ centers from low- to high-field type due to strong pressure-induced blue shift of the ⁴ T ₂ state, resulting in its crossing with the ² E state of Cr³⁺. This level-crossing effect was observed for the dominant Cr³⁺ _Li and Cr³⁺ _Nb centers at pressures that correlate well with estimations based on the ⁴ T ₂-² Eenergy gap (230 cm^-1 and 1160 cm^-1) and on the rate of their pressure-induced change (14.35 and 11.4 cm^-1/kbar, respectively). We also studied inhomogeneous broadeningof the ² E?⁴ A ₂transitions at ambient pressure for the minor high-field “defect” Cr³⁺ _Li centers in congruent LiNbO₃. A fine structure in the spectral response of these centers was observed. The obtained results are discussed on the basis of a microscopic hierarchic model for perturbed Cr³⁺ ions in the LiNbO₃ lattice. Received: 25 June 2001 / Published online: 2 November 2001     

Towards new lasers in Ti:Er:LiNbO3 waveguides: a study of the excited Er3+ states

Detailed excited state absorption measurements under pumping at 980 nm and 1.5 μm together with conventional absorption and emission spectroscopy is employed to investigate optical transitions of Er³⁺ in Ti:LiNbO₃ channel-waveguides. The experimental data were evaluated using the Judd–Ofelt method giving parameters close to those in the bulk. The good agreement between theoretical prediction and measurements allows us to calculate cross section, lifetimes, and branching ratios. Based on these results we developed and tested a model which is able to predict the conditions for which laser operation at 550 nm and 2.7 μm will be possible under 980 nm pumping. Received: 9 December 1998 / Revised version: 8 January 1999 / Published online: 24 March 1999     

Photorefractive properties of LiNbO3:Zn crystals related to the defect structure

LiNbO₃:Zn single crystals and powders were studied by precise X-ray diffraction methods. Structural refinement yielded new models of the intrinsic defect structure valid for different Zn concentration ranges. For concentrations up to 7 at. % in the crystal, Zn ions incorporate onto Li sites; at higher concentrations Zn ions are found on both Li and Nb sites. Photorefractive properties of LiNbO₃:Zn are discussed in the context of the deduced defect models. A smooth increase in the photoconductivity up to 7 at. % Zn is accounted for by a decrease of Nb antisites. Steeper growth of the photoconductivity at higher Zn concentrations is related to vanishing Li vacancies. Received: 17 November 2000 / Revised version: 23 January 2001 / Published online: 20 April 2001     

Thermal effect on multiphonon-assisted anti-Stokes excited upconversion fluorescence emission in Yb3+-sensitized Er3+-doped optical fiber

The temperature effect upon infrared-to-visible frequency upconversion fluorescence emission in Yb³⁺-sensitized Er³⁺-doped germanosilicate optical fibers excited with cw radiation at 1.064 μm is investigated. The experimental results revealed an eightfold enhancement in the visible upconversion emission intensity as the fiber temperature was increased from 17 °C to 180 °C. The fluorescence emission enhancement is attributed to the temperature-dependent multiphonon-assisted anti-Stokes excitation process of the ytterbium sensitizer. A theoretical approach that takes into account a sensitizer absorption cross-section, which depends on the phonon occupation number, has proven to agree very well with the experimental data Received: 6 April 1999 / Revised version: 27 August 1999 / Published online: 27 January 2000     

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.     

Spectroscopic and lasing properties of Er3+:Yb3+-doped fluoride phosphate glasses

Er³⁺ emission and lasing properties at 1.5 μm were studied in fluoride phosphate glasses (FP20) with different doping concentrations as well as in a commercial phosphate glass (Kigre QX). Emission decay behaviour at 1 μm and 1.5 μm was examined with respect to energy transfer between ytterbium and erbium. Emission cross-sections were determined using the reciprocity and Füchtbauer–Ladenburg methods. Gain spectra were calculated for the glasses and related to differences in the tuning curves and lasing properties. The temperature rise due to the quantum defect was determined via the ratios of green upconversion luminescence for different pump powers. The results from the laser and tuning experiments indicate that the FP20 glass offers good possibilities in broadband amplification and the generation of ultrashort pulses. Received: 24 August 2000 / Revised version: 27 October 2000 / Published online: 7 February 2001     

Raman characterization of H:LiNbO3 waveguides

In this work we present polarized Raman measurements of z-cut multimode H:LiNbO₃ waveguides in the κ_i- and β_i-phase states. A spectrum with unexpected form and behaviour, originating from the layer at the very surface, was observed in samples with various degrees of Li–H substitution. Possible reasons for the presence of this strange spectrum are considered. Received: 16 May 2001 / Revised version: 7 August 2001 / Published online: 23 October 2001     

NIR luminescence from Er/Yb, Tm/Yb, Er/Tm and Nd ions-doped zincborotellurite glasses for optical amplification

In this paper, we report the near-infrared luminescence from the Er³⁺/Yb³⁺, Tm³⁺/Yb³⁺, Er³⁺/Tm³⁺ and Nd³⁺ ions-doped TeO₂-ZnO-B₂O₃-Li₂O-Na₂O glasses for optical amplification. The X-ray diffraction (XRD) and differential scanning calorimetry (DSC) profiles of the host glass matrix have been carried out. From the DSC thermogram, glass transition (T_g), crystallization (T_c) and melting (T_m) temperatures have been evaluated. The near-infrared spectra of Er³⁺/Yb³⁺, Tm³⁺/Yb³⁺, Er³⁺/Tm³⁺ and Nd³⁺ ions-doped glasses have shown full-width at half-maxima (FWHM) around 58, 127, 87 and 35 nm, respectively. These glasses with better thermal stability and broad near-infrared emissions should have potential applications in broadly tunable laser sources and broadband optical amplification at low-loss telecommunication windows.     

Influence of Zn doping on electrooptical properties and structure parameters of lithium niobate crystals

We report the dependence of the unit cell parameters and the EO coefficients on Zn doping in optical-damage-resistant LiNbO₃:Zn crystals. Both properties depend in a non-monotonic manner on the Zn content. This is accounted for by different types of Zn ion incorporation into the lattice depending on the Zn concentration in the melt. Extrema observed in the concentration dependence of the EO coefficients at about 2–3 and 6.4 mol.% Zn correlate with an unusual concentration dependence of the unit cell parameters a and c. The low-concentration anomalies may be accounted for by a decrease of the Li vacancy concentration due to the Zn incorporation into Li sites. Anomalies at high concentrations are obviously due to a partial incorporation of Zn ions on Nb sites, which is reflected in the structure data. Anomalies in the concentration dependence of other optical properties at about 6–7 mol.% Zn reported recently are obviously related to a change in the localization of the Zn ions. The combination of high EO coefficients with a reduced optical damage for these concentrations make these crystals attractive for applications as Q-switching or electrooptical modulation. Received: 16 Nowember 1998 / Revised version: 8 December 1998 / Published online: 24 March 1999     

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     

Effect of stresses on the OH libration bands in proton-exchanged LiNbO3 optical waveguides

i -H_xLi_1-xNbO₃ phases generated on x-cut LiNbO₃ the new anisotropic libration mode at 890–940 cm^-1 is observed in addition to the known isotropic mode at 960–970 cm^-1, whereas the same phases on z-cut exhibit only latter isotropic libration mode. The observed phenomena are explained as a result of anisotropic stresses generated in the x-cut waveguides, whereas the stresses in the structures on z-cut are isotropic. The OH-bond librations are clearly anisotropic in the α, κ₁, and κ₂ phases generated on both z- and x-cuts, which indicates a fundamental difference of the local symmetry of the proton’s position in the β_i phases compared to the α, κ₁, and κ₂ H_xLi_1-xNbO₃ phases. Received: 4 May 1998/Revised version: 26 June 1998