Laser induced memory bits in photorefractive LiNbO3 and LiTaO3

We study experimentally the formation of refractive index voxels (volume elements) in photorefractive LiNbO₃ and LiTaO₃ crystals illuminated with high irradiance femtosecond laser pulses. We used 150 fs pulses at 800 nm wavelength (energy 6–50 nJ) tightly focused inside the crystals in a single shot regime. This resulted in a formation of a micrometer size region of elevated refractive index, which may be used as memory bits in information storage/retrieval application. The maximum refractive index change of 5×10⁻⁴ was recorded in undoped LiNbO₃ at an average light intensity of ∼TW/cm² that is close to the breakdown threshold. A simple setup for photorefractive recording and in situ monitoring of the refractive index changes has been proposed. M. Sūdžius leaves from: the Institute of Materials Science and Applied Research of Vilnius University, Lithuania.     

LiTaO3 as holographic storage material

The optical storage properties of LiTaO₃:Fe are investigated and compared with those of the isomorphous compound LiNbO₃:Fe. Absorption, photocurrent, photoconductivity and holographic measurements are reported. In the case of photovoltaic writing similar results for LiTaO₃- and LiNbO₃-crystals are obtained. However, in the case of photoconductive writing using external electric fields LiTaO₃:Fe-crystals yield much better results due to large photoconductivity values. Considering the recording sensitivity and the extremely large storage time LiTaO₃:Fe turns out to be one of the most promising materials for photorefractive storage of volume phase holograms.     

Optical properties of Tm,Mg:LiTaO3 laser crystal

A Tm, Mg co-doped LiTaO₃ crystal has been grown by Czochralski method. Room temperature polarized absorption spectra and fluorescence spectrum of the Tm, Mg:LiTaO₃ crystal were measured and analyzed. The maximum absorption cross-section is 6.0791 × 10⁻²⁰ cm² at around 790 nm with full width at half maximum of 5 nm. The emission cross-section of ³ F ₄ manifold was 2.2 × 10⁻²⁰ cm². The spectroscopic parameters of Tm³⁺ ion were calculated by applying the Judd-Ofelt approach, and the intensity parameters Ω₂, Ω₄, and Ω₆ were obtained to be 7.71 × 10⁻²⁰, 1.09 × 10⁻²⁰, and 1.16 × 10⁻²⁰ cm², respectively. The branching ratios and radiative lifetimes were also presented and the radiative lifetime of Tm^{3+ 3} F ₄ → ³ H ₆ transition is 968.3 μs. The results were also analyzed and compared with other Tm³⁺ doped hosts.     

Growth and optical properties of Mg, Fe Co-doped LiTaO3 crystal

Mg, Fe double-doped LiTaO₃ and LiNbO₃ crystals have been grown by Czochralski method. The optical properties were measured by two-beam coupling experiments and transmitted facula distortion method. The results showed that the photorefractive response speed of Mg:Fe:LiTaO₃ was about three times faster than that of Fe:LiTaO₃, whereas the photo-damage resistance was two orders of magnitude higher than that of Fe:LiTaO₃. In this paper, site occupation mechanism of impurities was also discussed to explain the high photo-damage resistance and fast response speed in Mg:Fe:LiTaO₃ crystal.     

Determination of the absorption constant in the interband region by photocurrent measurements

We determined high absorption constants of crystals from photocurrent measurements within the interband absorption region (10–10⁴ cm^-1). The method has been demonstrated in the interband absorption regime near 530 nm in Sn₂P₂S₆, a novel infrared sensitive photorefractive material, and in the interband absorption regime near 257 nm of near stoichiometric LiTaO₃. Besides the verification of older measurements with our new technique, precise absorption data for Sn₂P₂S₆ in the wavelength range 488–514 nm are presented. PACS 42.70.Nq; 72.41.+w; 78.20.Ci     

The nonlinear optical property and photoinduced anisotropy of?a?novel azobenzene-containing fluorinated polyimide

A novel azobenzene-containing fluorinated polyimide was synthesized. The nonlinear optical property and photoinduced birefringence of a polyimide thin film were investigated. Large third-order nonlinear refraction (n ₂=−4.49×10⁻¹¹ cm²/W) was observed in the polyimide thin film by carrying out Z-scan measurement. The polyimide thin film exhibited larger nonlinear refraction than that of a mono-azo dye doped PMMA thin film (n ₂=−1.63×10⁻¹² cm²/W). The photoinduced birefringence of the polyimide thin film (▵ n∼10⁻²) under different pump intensities was investigated; it was much larger than that of the mono-azo dye doped PMMA thin film (▵ n∼10⁻³). Moreover, the time constants for birefringence growth and relaxation processes were determined.     

Photorefractive waveguides in oxide crystals: fabrication, properties, and applications

3 , LiTaO₃, BaTiO₃, KNbO₃, Sr_xBa_1-xNb₂O₆ (0.25≤x≤0.75, SBN), and Bi₁₂(Si,Ti,Ge)O₂₀ (BSO, BTO, BGO) waveguides are discussed. Furthermore, the suitability of photorefractive waveguides for nonlinear optical components is demonstrated in some examples. Received: 21 April 1998/Revised version: 28 May 1998     

Thermo-optic effects in electro-optic crystals used in an intensity-modulation system. – Application in LiTaO3

Linear electro-optic (EO) and thermo-optic (TO) effects are jointly considered on the basis of field-induced and temperature-affected perturbations of the operating point along the optical transmission curve of an EO-modulation system. In this framework, methods of EO measurements based on the frequency doubling appearing at the minimum-transmission point are formulated. Moreover, TO coefficients for various optical quantities, such as the refractive indices, n₀ and n_e, the spontaneous birefringence Δn⁽⁰⁾, the EO coefficient r, the half-wave voltage V_π, the optical phase retardation Γ, and the intensity modulation (IM) depth, m, are introduced and useful relationships between them are extracted. Also, applications of the above in the experimental field, with determinations of EO parameters and TO coefficients, are presented for the case of a congruent LiTaO₃ crystal. A comparison of the so-obtained experimental results with those derived from literature when a LiNbO₃ crystal is used demonstrates a number of advantages for the LiTaO₃-based system. PACS 78.20.Jq; 65.40.De     

Proton-exchange influence on the polar phonons of LiTaO3 optical waveguides

Refractive index change and Raman scattering of Z-cut proton-exchanged LiTaO₃ optical waveguides with different composition have been studied. Probing of the waveguide depth was carried out by using micro-Raman spectroscopy in order to distinguish layers with different phase states. Varying the proton-exchange and post-exchange annealing regimes, two phases –α and β– in addition to the pure LiTaO₃, were clearly observed. The behaviour of the A ₁ vibrations of the TaO₆ groups was found to be very sensitive to the phase changes. Using data from waveguide Raman spectra, normal and oblique E(TO, LO) phonons were sorted and their properties were followed in the α and β phases. The OH-stretchings are considered to correspond to dipoles turned out of the oxygen planes. Received: 9 July 1999 / Accepted: 11 October 1999 / Published online: 24 March 2000     

Growth and photorefractive properties of near-stoichiometric In:Fe:Cu:LiNbO3 crystals

The near-stoichiometric LiNbO₃ crystal co-doped with In₂O₃, Fe₂O₃, and CuO has been grown from a Li-rich melt (Li/Nb = 1.38, atomic ratio) by the Czochralski method in air atmosphere for the first time. The OH⁻ absorption spectra were characterized to investigate the structure defects of the crystals. The appearance of the 3506 cm⁻¹ absorption peak manifests that the composition of the grown crystal is close to the stoichiometric ratio. The photorefractive properties were also measured by the two-wave coupling experiments. The results show that the near-stoichiometric In:Fe:Cu:LiNbO₃ crystal has a larger refractive index change, higher recording sensitivity and larger two-wave coupling gain coefficient than those obtained in the congruent In:Fe:Cu:LiNbO₃ crystal under the same experimental conditions. The material of near-stoichiometric In:Fe:Cu:LiNbO₃ crystal is a promising candidate for blue photorefractive holographic recording.     

Electron paramagnetic resonance studies in photorefractive crystals I: Hyperfine interaction and photoinduced charge transfer in233U5+ and238U5+ doped LiNbO3

Electron paramagnetic resonance studies were conducted on the photoinduced charge transfer and also hyperfine interaction of U⁵⁺ stabilized in photorefractive matrix LiNbO₃. This work deals with: (i) first observation of hyperfine structure due to²³³U (I=5/2) in its pentavalent state at octahedral sites and comparison with other possible site symmetries, (ii) photoinduced charge transfer as observable by EPR and its relevance to photorefractive behaviour of LiNbO₃. The effect of chemical bonding on the hyperfine interaction of 5f ¹ configuration was also studied by converting the existing literature data on²³⁵U⁵⁺ to that of²³³U⁵⁺ by standard methods. This suggests that progressive substitution of oxygen by F⁻, in the series UO ₆ ⁷⁻ , (UO₅F)⁶⁻ and (UO₄F₂)⁵⁻ drastically decreases the hyperfine coupling constantA _∥, along the local distortion axis. This trend is explained as being due to the absence of ligand ion along the distortion axis at U⁵⁺ site in trigonal LiNbO₃. The effects of illumination by copper vapor laser (CVL) on the intensity of the U⁵⁺ signal was studied in the 10–300K region. The kinetics of decay and restoration of U⁵⁺ was also studied between 10–100K range. The decay kinetics was found to obey double exponential. The reduction of concentration of U⁵⁺ with CVL-illumination and its restoration in the absence of light show that pentavalent uranium takes part in the photorefractive effects in LiNbO₃.     

Photorefractive centers in LiNbO3, studied by optical-, Mössbauer- and EPR-methods

The photorefractive properties of LiNbO₃∶Fe and LiNbO₃∶Cu have been studied in combination with optical absorption-, Mössbauer- and EPR-measurements. The charge states of Fe in successively reduced LiNbO₃∶Fe have been investigated with respect to the influence on the photorefractive sensitivity and saturation value of the refractive index change. The results of this experiment demonstrate clearly the close correlation between the concentration of Fe²⁺ impurities and the optical absorption band around 2.6 eV in LiNbO₃∶Fe, which is known to give rise to an anisotropic charge transport upon optical excitation. The resulting photocurrents determine the photorefractive sensitivity mainly in the initial state of halographic exposure. With increasing conversion from Fe³⁺ to Fe²⁺ the photorefractive sensitivity saturates and the saturation value of the refractive index change decreases remarkably. In the case of LiNbO₃∶Cu a similar behaviour of the photorefractive storage parameters after successive reduction treatments has been observed qualitatively. However, in contradiction to LiNbO₃∶Fe the Cu²⁺ centers cannot be related to the photorefractive sensitivity of LiNbO₃∶Cu. These results are discussed with respect to the predictions of two models concerning the microscopic nature of the photorefractive process in doped LiNbO₃.     

Positronium interactions with Cu(II) Ions in water

Summary Positronium reactions with Cu(II) ions in aqueous solution were investigated by measuring the concentration dependence of lifetime spectra and of 1D-ACAR curves for the following Cu (II) complexes: [Cu(H₂O)₆[²⁺, [Cu(NH₃)₄ (H₂O)₂]²⁺ and [Cu(EDTA)(H₂O)]²⁻. The combined analysis of lifetime and ACAR data shows that Cu(II) ions:a) reduce the formation of positronium (inhibition effect),b) promote both ortho ⇌ para conversion and redox reactions. It was also found that inhibition and reaction rate constants are affected by the ligand type.     

The nonlinear optical susceptibility and electro-optic tensor of ferroelectrics: first-principle study

The nonlinear optical properties of some ABO₃ materials (BaTiO₃, KNbO₃, LiTaO₃ and LiNbO₃) are studied by density functional theory (DFT) in the local density approximation (LDA) expressions based on first-principle calculations. Our goals are to give the details of the calculations for linear and nonlinear optical properties, including the linear electro-optic (EO) tensor for some ABO₃ structures with oxygen octahedral structures using first-principles methods. These results can then be used in the study of the physics of ferroelectrics, specifically, we present calculations of the second harmonic generation response coefficient X _ijk ⁽²⁾ (−2ω, ω, ω) over a large frequency range for ABO₃ crystals. The electronic linear EO susceptibility X _ijk ⁽²⁾ (−ω, ω,0) is also evaluated below the band gap. These results are based on a series of the LDA calculations using DFT. Results for X _ijk ⁽²⁾ (−ω, ω,0) are in agreement with experiments below the band gap. The results are compared with the theoretical calculations and the available experimental data.     

Crystal growth and spectroscopic characterization of Yb:LiTaO3

Spectroscopic properties are presented for Yb³⁺ incorporated into single crystals of LiTaO₃ grown by the top-seeded solution growth method. From an analysis of the absorption and fluorescence spectra, we are able to determine the Stark-level components of the ²F_7/2 (the ground-state multiplet manifold) and the ²F_5/2 (the excited-state multiplet manifold of Yb³⁺ (4f¹³)). The room-temperature fluorescence lifetime of ²F_5/2 is 678 μs as measured on a thin sample to reduce possibilities for reabsorption. Spectral comparisons of Yb³⁺-doped LiTaO₃ and LiNbO₃ are drawn. The crystal-field splitting of Yb³⁺(4f¹³) in both crystal hosts is modeled using a set of crystal-field splitting parameters, B_nm, determined from a recent spectroscopic analysis of Er³⁺(4f¹¹) in LiNbO₃. Without adjustment of the B_nm parameters, the model predicts the Stark-level energy and the symmetry label for each level in reasonable agreement with the experimental values. Less photorefractive than its niobate cousin, LiTaO₃ has potential for use in numerous integrated electro-optical circuits and devices.     

Radio-frequency absorption study of the parameters of high-T c materials irradiated with fast reactor neutrons

The magnetic properties of YBa₂Cu₃O_7−x ceramics of various densities and Bi₂Sr₂CaCu₂O₈ quasicrystals irradiated with neutrons at fluences of 10¹⁶–10¹⁹ cm⁻² are investigated by a radio-frequency method (in the frequency range f=100–150 MHz). The electromagnetic absorption is used to estimate the parameters of a Josephson medium: the lower critical field, the critical current density, the grain size and intergranular distances, and the penetration depth of the magnetic field in the sample. The hysteresis of electromagnetic absorption in the indicated superconductors is investigated; the hysteresis effect can be used to obtain data on flux pinning processes and flux creep dynamics. It is shown that an increase in the critical current density is observed as a result of the injection of radiation-induced pinning centers. Fiz. Tverd. Tela (St. Petersburg) 39, 28–34 (January 1997)     

Electron spin resonance of copper pair centers in crystals with perovskite structure

Copper pair centers, which could be of interest for obtaining quantitative information about exchange interactions in superconductors based on cuprate perovskites, are observed in crystals with the perovskite structure by the ESR method. Such centers are investigated in KTaO₃:Cu and K_1−x Li_xTaO₃:Cu crystals. A model consisting of a chain of two equivalent Cu²⁺ ions and three oxygen vacancies, extending along the 〈 100〉 axis, is proposed for the centers. The exchange interaction in the pairs is ferromagnetic. Pis’ma Zh. éksp. Teor. Fiz. 69, No. 12, 890–894 (25 June 1999)     

Z-scan measurements of photorefractive nonlinearities for a SBN: Ce crystal

 In this paper, we derived the Z-scan formula for a photorefractive crystal sample under an external applied electric field. The far-field diffraction pattern of a Gaussian beam wavefront through a photorefractive crystal is calculated by considering spatial-phase perturbation induced by the space-charge field. The photorefractive drift nonlinearities and correspondingly, the electro-optic coefficients r ₃₃, r ₁₃, (r ₂₃) and the characteristic ratio n ³ _e r ₃₃/n ³ _o r ₁₃ for a cerium-doped Sr_0.61Ba_0.39Nb₂O₆ crystal are determined from the Z-scan experiments. Z-scan with enhanced sensitivity is also realized by measuring the normalized transmittance at the off-axis position in the far field. A deviation between the off-axis Z-scan experimental results and the theoretical prediction is discussed too. Received: 22 July 1996/Revised version: 7 October 1996     

Enhancement of nonvolatile blue photorefractive properties in LiNbO<Subscript>3</Subscript>:In:Fe:Cu crystals

The nonvolatile photorefractive characteristics of LiNbO₃:Fe:Cu and In-doped LiNbO₃:Fe:Cu crystals are investigated. The stronger nonvolatile blue photorefraction observed can be ascribed to its remarkable characteristic of being in phase between the two gratings recorded in shallow and deep trap centers, which is one or two orders of magnitude higher than those obtained in conventional two-color recordings under the same recording conditions. Furthermore, it is interesting that, compared with LiNbO₃:Fe:Cu, the recording properties, such as the saturation refractive index change, nonvolatile sensitivity and response time at 488 nm wavelength are enhanced in LiNbO₃:In:Fe:Cu crystals under the same recording conditions. The so-called damage-resistant dopants such as In³⁺ ions in red photorefraction are not damage resistant at 488 nm wavelength but they enhance the blue photorefraction. PACS  42.40.Ht; 42.40.Lx; 42.70.Ln     

Metastable phases in HxLi1-xTaO3 waveguide layers and pure LiTaO3

The formation of high-temperature phases in low-doped H:LiTaO₃ waveguide layers in Z-cut LiTaO₃ has been observed both by refractive-index and IR-spectra measurements. This permits us to correlate the index jumps to the changes of the OH bonds in the crystal lattice. Reversible phase transitions were detected in the temperature interval T=50–200 °C over a wide range of hydrogen content including as-grown LiTaO₃. The high-temperature phases are metastable close to room temperature. This was demonstrated by tracing the time evolution of the refractive-index change. It was shown that the high-temperature phases are responsible for the long-term refractive-index instabilities in both H:LiTaO₃ waveguides and virgin LiTaO₃. Received: 7 May 2001 / Revised version: 10 August 2001 / Published online: 30 October 2001