X-ray-induced photochromic effects in copper-doped lithium niobate crystals

X-Ray-induced absorption changes in Cu-doped lithium niobate crystals (LiNbO₃) are investigated. All induced photochromic effects are fully reversible, i.e., illumination with white light annihilates the absorption changes. With increasing doping level, a decrease in the saturation value of the absorption changes is found. Changes of the Li concentration of the crystal to a more stoichiometric composition via Li indiffusion further decreases the photochromic effect. For sufficient X-ray doses, the saturation value is independent of the radiation energy in the measured range from 50–150 kV. The spectral distribution of the X-ray-induced absorption changes and the slow dark decay indicate that the additional absorption results from an increase of the Cu⁺ concentration. Received: 20 December 2000 / Revised version: 24 January 2001 / Published online: 27 April 2001     

Dark conductivity in copper-doped lithium niobate crystals

The impact of protons and copper on the dark conductivity of copper-doped photorefractive lithium niobate crystals is investigated by observation of the dark decay of holograms. The dark conductivity is significantly smaller than that of iron-doped lithium niobate. A non-mono-exponential hologram decay is observed, which needs to be considered for multiplexing of holograms. Received: 25 March 2002 / Published online: 2 May 2002     

Electrooptic properties of lithium niobate crystals for extremely high external electric fields

The electrooptic effect in lithium niobate crystals (LiNbO₃) for extremely high externally applied electric fields of up to 65 kV/mm is investigated. Homogeneous electrooptic refractive-index changes of up to 4.8×10^-3 are found for ordinarily polarized light. No quadratic electrooptic effect is observed. An upper bound for the quadratic electrooptic coefficient of |s₁₃|≤2.3×10^-21 m²/V² is determined. Electrooptic, angular, and wavelength tuning of the Bragg condition of a thermally fixed hologram are demonstrated. Received: 29 October 2002 / Revised version: 14 January 2003 / Published online: 26 March 2003 RID="*" ID="*"Corresponding author. E-mail: ml@uni-bonn.de     

Effect of annealing on the electrical properties and refractive index of HgI2 single crystals

The effect of annealing on the electrical properties and the refractive index of red mercuric iodide (HgI₂) single crystals is investigated. The ac-impedance and phase angle were measured in the frequency range from 100 Hz to 10 kHz at different annealing temperatures. The ac-conductivity, dielectric constants, loss tangent and the refractive index as a function of frequency are determined. The results are discussed in terms of structural changes taking place as a result of the heat treatment of the HgI₂ single crystals.     

Photorefractive properties of highly-doped lithium niobate crystals in the visible and near-infrared

Light-induced refractive-index changes, bulk-photovoltaic current densities, and photoconductivities of photorefractive iron-doped lithium niobate crystals (iron concentrations between 0.02 and 0.17 wt. %) are investigated in detail using visible and near-infrared light. It turns out that the one-center model predicts the material performance correctly for small iron concentrations (c_Fe<0.06 wt. % Fe₂O₃), only. A strong increase of the photoconductivity for higher doping levels limits the space-charge fields. Refractive-index changes up to 7×10^-4 for green and 2.8×10^-4 for near-infrared ordinarily polarized light are obtained. The corresponding hologram multiplexing numbers are 11 for green and 5 for near-infrared light. Received: 18 November 1998 / Revised version: 8 January 1999 / Published online: 7 April 1999     

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     

Poling dynamics of lithium niobate crystals

Ferroelectric domain reversal via electric field poling of congruently melting lithium niobate (LiNbO₃) crystals is investigated. An electro-optic interferometric observation technique reveals spatial and temporal dynamics of the poling process. Starting from seeds, the domains grow until the entire crystal has a switched polarization. During the switching process the boundaries are preferentially aligned along the crystallographic axes. The coercive field between two sequenced domain inversions is transiently reduced after a poling event, and recovers exponentially with a time constant of about half a minute. No light-induced change of the recovery time constant, neither with green nor with ultraviolet light, is observed. The results are of relevance for domain engineering of LiNbO₃ crystals. Received: 6 February 2003 / Published online: 9 April 2003 RID="*" ID="*"Corresponding author. Fax: +49-228/734038, E-mail: wengler@physik.uni-bonn.de     

Thermal lens spectrometry in pyroelectric lithium niobate crystals

In this work, the light-induced lens effect due to thermal and/or photorefractive processes was studied in pyroelectric (undoped and Fe²⁺-doped) lithium niobate crystals (LiNbO₃) using thermal lens spectrometry with a two-beam (pump–probe) mode-mismatched configuration. The measurements were carried out at two pump beam wavelengths (514.5 and 750 nm) to establish a full understanding of the present effects in this material (thermal and/or photorefractive). We present an easy-to-implement method to determine quantitative values of the pyroelectric coefficient (dP _s/dT), its contribution to the thermal effect and other thermo-optical parameters like thermal diffusivity (D), thermal conductivity (K) and temperature coefficient of the optical path length change (ds/dT). These measurements were performed in LiNbO₃ and LiNbO₃:Fe (0.1 ppm Fe²⁺) crystals with c axis along the direction of laser propagation.     

Electro-optic and dielectric properties of Hafnium-doped congruent lithium niobate crystals

We report the optical and dielectric properties in hafnium (Hf)-doped lithium niobate (LN) crystals. We investigated samples of congruent composition with various doping concentration varying from 0 to 8 mol%. The clamped and unclamped values of the electro-optic coefficient r ₂₂ of Hf-doped LN and the corresponding dielectric permittivity as well, have been experimentally determined and compared with the results obtained in undoped congruent LN crystals. We show that the electro-optic and dielectric properties are only slightly affected by the introduction of hafnium ions, and therefore Hf-doped LN has the advantage of low photorefractive damage compared with the undoped congruent LN.     

Interrelation of intrinsic and extrinsic defects – congruent, stoichiometric, and regularly ordered lithium niobate

A new approach to the intrinsic and extrinsic defect subsystems, considering them as one integrated functional system, is developed for complex oxides. The strong interrelation of these subsystems becomes especially apparent when concentrations of both defect classes are comparable. A new parameter, reflecting the total intrinsic defect concentration, is introduced to determine the degree of crystal imperfection. The necessity of at least two calibrated samples – congruent and regularly ordered crystals – is substantiated. The accuracy by which the parameter can be determined can serve as a criterion in comparison of different methods of crystal characterisation. A procedure for crystal calibration by several physical characteristics is illustrated. Such a heuristic generalisation of the concept of mutual correlation of the whole defect system and the material only became possible on the basis of experimental and theoretical study of large numbers of LiNbO₃ crystals. The spectra of EPR, NMR, ENDOR, and other properties of crystals with different compositions, diverse modifiers (K, Mg,...), and various probe impurities have been analysed. It is found that crystals with vanishingly small concentration of intrinsic defects offer extraordinary informative opportunities. Their micro- and macroscopic properties are discussed. The developed ideas have a general character; therefore they should also be valid for other non-stoichiometric complex oxides. Received: 3 December 1998 / Revised version: 15 February 1999 / Published online: 12 April 1999     

Tailoring the nonlinear refractive index of fluoride-phosphate glasses for laser applications

In this paper we report on measurements of the nonlinear refractive index n₂ at 1047 nm of various fluoride-phosphate laser glasses relative to fused silica using degenerate four-wave mixing. We find good agreement with empirical estimates obtained from the d-line linear refractive index and the Abbe number for pure fluoride-phosphate glasses. Significant increase of n₂ is observed when adding sulfate and niobium oxide to the glass composition offering tailorable nonlinear properties for glasses employed in short pulse laser oscillators. Received: 27 December 1999 / Published online: 24 March 2000     

Influence of optical-damage-resistant dopants on the nonlinear optical properties of lithium niobate

Using the chemical-bond method, nonlinear optical properties of lithium niobate containing different dopants are calculated. In crystals with stoichiometric composition the second order nonlinear susceptibility decreases approximately linearly with increasing dopant concentration. Among the dopants studied – Mg, Zn and In – this behaviour is most highly expressed for In doping. In contrast to that, congruently grown crystals show a different behaviour; only a weak dependence on the dopant concentration is found for, for example, Mg-doped material. Received: 24 October 2000 / Published online: 21 March 2001     

Simulation of refractive index profiles for titanium indiffused lithium niobate channel waveguides

A generally applicable method to simulate the two-dimensional profiles of Ti-concentration and refractive index of Ti:LiNbO₃, waveguides is presented. The influence of the fabricational parameters on the refractive index profiles has been studied in detail. The model parameters are extracted from the available experimental data. The computed values of surface refractive index change agree closely with the experimental results. The model is also extended for coupled waveguides.     

Beam-coupling in tetragonal potassium Tantalate-Niobate crystals

Beam-coupling is investigated in a nominally pure tetragonal potassium Tantalate-Niobate (KTN) crystal as a function of external electric field, spatial frequency and light wavelength. The variation of these parameters leads to a change of the direction of energy transfer between the two recording beams. The experimental results can be consistently described by a one-center charge-transport model taking into account electron and hole contributions to photoconductivity and space-charge limitations due to the available trap density.     

Etch frustration in congruent lithium niobate single crystals induced by femtosecond ultraviolet laser irradiation

Modification of the chemical etching behaviour of undoped congruent z-cut lithium niobate single crystals is achieved by pre-illumination of the –z face of the crystal with sub-ps ultraviolet laser radiation at 248 nm, at energy fluences below the threshold for ablation. A systematic study of the effect of the energy fluence and total exposure on the etch frustration is presented. Received: 23 July 2001 / Accepted: 28 September 2001 / Published online: 20 December 2001     

Electrical fixing of waveguide channels in strontium-barium niobate crystals

We demonstrate a new method of electrical fixing of waveguiding channels in strontium-barium niobate. The method is applicable to both bulk material and planar SBN waveguides. Waveguiding is achieved for extraordinarily polarized light. We suggest that the fixing is based on a partial depoling of the crystal rather than on internal electric fields. Received: 29 January 2001 / Published online: 27 April 2001     

Two-wave mixing bistability based on mixed grating formation in photorefractive crystals

1 L) and the relative strength (x) of PCG compared with PRG in two cases: (i) when g₁L>0 and x>1 so that there exists either pure PRG or PRG dominates over PCG, and (ii) when g₁L<0 and x<-1 so that there exists either pure PCG or PCG dominates over PRG. The threshold condition g₁L>(g₁L)_Th=2x(1+1/R) with R>1 and the effective coupling strength, g₂L=g₁L/x>0 with 1<x<-1, need to be satisfied for the bistability. Possible regions of bistability affect the position of the region for the intensity ratio (m) of the incident beams where two branched multiple solutions exist and hysteresis in the gain is expected. Gain solutions are found to be single valued without bistability when g₂L<0. A comparison between the mixed grating gain and pure PRG/PCG gains with the occurance of bistability is presented and interpreted physically. Received: 9 January 1996/Revised version: 17 September 1996     

The aging effect on the dispersion of the refractive index of lithium fluoride in the wavelength range of 460–1000 nm

Transmittance measurements were carried out for LiF thin films directly after preparation, then one day, one week, four weeks and six weeks later. The aging effect on the optical properties of the film was thus studied. This showed that the aged LiF films have refractive indices larger than those of fresh films.     

Influence of oxidation on optical diffuse reflectance spectra in nanoscale silicon powder

Received: 5 June 1997/Accepted: 30 July 1997