Gap levels of Ti<Superscript>3+</Superscript> on Nb or Li sites in LiNbO<Subscript>3</Subscript>:(Mg):Ti crystals and their effect on charge transfer processes

The Ti dopant occupying Li or Nb sites and the charge transfer processes induced by thermochemical reduction and optical bleaching treatments have been investigated in LiNbO₃ systems using optical absorption and EPR. The Ti³⁺ centers, built preferentially at Nb sites in heavily Mg-codoped crystals, are shown to have absorption bands at 1.62±0.08 eV and 2.65±0.25 eV, which are similar or slightly redshifted compared to Ti³⁺ centers at Li sites in LiNbO₃:Ti crystals. The Ti_Nb^4+/3+ gap level plays an important role in the trapping of electron-polarons in LiNbO₃, double-doped with Mg and Ti; in particular, an enhanced optical detrapping sensitivity for pumping in the 1.3–2.8 eV range is observed, which may be relevant for applications in integrated optics. Evidence indicating the possible existence of bipolarons involving the Ti dopant is presented. PACS 77.84.Dy; 71.55.Ht; 71.38.-Mx; 78.40.Ha; 76.30.Fc     

Dispersion of the dielectric function real part for Mg:LiNbO3 crystals at terahertz frequencies

We study dispersion of the dielectric function real part ε′ in the terahertz-frequency range for bulk and periodically poled congruent LiNbO₃ and Mg:LiNbO₃ crystals. The concentration of Mg in Mg:LiNbO₃ samples was close to 5 mol%, which is the photorefractive threshold. Approximate expressions for extraordinary polariton dispersion dependence were obtained in the range 0.5–6.5 THz. The influence of Mg-dopant on the optical properties of crystals in the terahertz range is revealed. Changes of the defect structure of lithium niobate crystals are discussed.     

Ultraviolet photorefractive effect in Mg-doped near-stoichiometric LiNbO3

The ultraviolet photorefractive effect of Mg-doped near-stoichiometric LiNbO₃ crystals prepared by vapor transport equilibration (VTE) technique was studied at 351 nm. It was found in the near-stoichiometric LiNbO₃ crystals that the ultraviolet photorefractive effect could be enhanced greatly with the increase of Mg concentration. Based on the activation energy of dark decay of the photorefractive grating, possible centers responsible for the ultraviolet photorefractive effect were also discussed.     

Optical waveguides in LiNbO<Subscript>3</Subscript> and stoichiometric LiNbO<Subscript>3</Subscript> crystals by proton exchange

The formation of optical planar waveguides in LiNbO₃ and stoichiometric LiNbO₃ crystals by proton exchange was reported. The prism-coupling method was used to characterize the dark-line spectroscopy at the wavelength of 633 and 1539 nm, respectively. The mode optical near-field outputs from proton-exchanged LiNbO₃ and SLN waveguides at 633 nm were presented. The mode field from stoichiometric LiNbO₃ (SLN) waveguide is lighter and more uniform than that from LiNbO₃ waveguide, which means the quality of the waveguide in SLN crystal is better than that of the LiNbO₃ waveguide. For proton-exchanged LiNbO₃ waveguides, the evolution of the refractive index profile with annealing was presented. The disorder profiles of Nb atoms in proton-exchanged LiNbO₃ waveguides were obtained by Rutherford backscattering/channeling technique. It is shown that the longer the exchange time, the larger the displacement of Nb atoms. Supported by the National Natural Science Foundation of China (Grant No. 10475052) and the Scientific Research Start-up Financing of Qufu Normal University     

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     

The effect of In doping on optical properties of Fe:LiNBO3 crystals

Fe:LiNbO₃ and In:Fe:LiNbO₃ crystals were grown by Czochralski method. The absorption spectra were measured to investigate their defect structure. The photo damage resistance and photorefractive properties were measured. The photo damage resistance of the In:Fe:LiNbO₃ crystal in which the In concentration is above the threshold value is one order of magnitude higher than that of the Fe:LiNbO₃ crystal. The mechanisms of the violet shift of the absorption edge and the enhancement of the photorefractive effect of In:Fe:LiNbO₃ crystals were investigated.     

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.     

Optical properties of LiNbO3:Mg(5.21 mol %) and LiNbO3:Fe(0.009 mol %):Mg(5.04 mol %) crystals

Using methods of electronic spectroscopy, laser conoscopy, photoinduced (photoreactive) light scattering, and Raman light-scattering spectroscopy, we have studied the optical homogeneity, optical transmission, and photorefractive properties of single crystals LiNbO₃:Mg(5.21 mol %) and LiNbO₃:Fe(0.009 mol %):Mg(5.04 mol %) that were grown from congruent melts. We have ascertained that doping with “nonphotorefractive” Mg²⁺ cations causes suppression of the photorefractive effect in a lithium-niobate crystal. Upon double doping (Fe:Mg), if the concentration of Mg²⁺ cations exceeds the threshold concentration, the photorefractive effect is almost not observed and the presence of “photorefractive” Fe cations does not affect the photorefractive effect as strongly as in congruent crystals doped with Fe.     

Selective photorefractive scattering in LiNbO<Subscript>3</Subscript>:Rh crystals

Photorefractive scattering occurs in rhodium-doped lithium niobate crystals irradiated by coherent light. The photorefractive scattering has both wide-angle and selective components. The results of experimental investigation of selective photorefractive scattering in LiNbO₃:Rh crystals and calculation of the spatial structure of scattering are reported. The selective scattering is regarded as a kind of a frequency-degenerate fourwave vector interaction.     

Defect structure and optical damage resistance of Zn:Fe:LiNbO<Subscript>3</Subscript> crystals

A series of Zn:Fe:LiNbO₃ crystals were prepared by the Czochralski technique with 0.015 wt. % Fe₂O₃ content and various concentrations of ZnO. The ultraviolet-visible absorption spectra and the infrared absorption spectra of the Zn:Fe:LiNbO₃ crystals were detected in order to investigate their defect structure. Their optical damage resistance was characterized by the photoinduced birefringence change and transmission facula distortion method. The optical damage resistance of the Zn:Fe:LiNbO₃ crystals increases remarkably when the concentration of ZnO is over its threshold concentration (more than 6.0 mol. %). The effects of defects on the optical damage resistance of the Zn:Fe:LiNbO₃ crystals are discussed in detail. Received: 25 October 2002 / Revised version: 6 January 2003 / Published online: 22 May 2003 RID="*" ID="*"Corresponding author. Fax: +86-451/2300-926, E-mail: zzxxhhdoctor@sina.com     

Polarons in magnesium-doped lithium niobate crystals induced by femtosecond light pulses

Strong light-induced absorption has been observed in lithium niobate crystals doped with magnesium after application of femtosecond illumination. In this material there are no Nb-on-Li-site defects and hence no antisite polarons occur, but small free polarons close to the conduction band can be generated. The light-induced absorption observed is attributed to these polarons. For LiNbO₃:Mg, their decay times are about two orders of magnitude smaller than those of the Nb-on-Li-site polarons in undoped material. The results are relevant for a better understanding of the suppression of the so-called optical damage in these crystals and for their use in femtosecond applications.     

Generation of small bound polarons in lithium niobate crystals on the subpicosecond time scale

Light pulses of 240 fs duration and 388-nm wavelength generate in lithium niobate crystals transient absorption. The absorption changes are observed with delayed ultra-short pulses (wavelength 776 nm) and with continuous-wave light (wavelength 785 nm) over 10 decades from 400 fs up to 10 s after the pump pulse. The decay is well described by one stretched-exponential function over the entire temporal range. We attribute the absorption changes to small bound polarons because of the temporal, spectral, and polarization fingerprints. The polarons are formed in less than 400 fs after the pump illumination, ruling out that phonons with wavenumbers below 100 cm^-1 are the main cause for polaron generation and indicating that the breathing mode of the oxygen octahedra is of relevance. An upper limit of the generated polaron concentration is estimated as ≈4.4×10¹⁸ cm^-3 with an intensity of ≈220 GW/cm². PACS 71.38.Ht; 78.47.+p; 77.84.Dy; 42.50.Gy; 42.70.Mp; 72.20.Jv     

Specific features of growth and structure of LiNbO<Subscript>3</Subscript> : Zn crystals near the ZnO concentration threshold of 6.76 mol %

The crystallization conditions and Raman spectra of LiNbO₃ : Zn crystals (0.02–8.91 mol % ZnO in the melt) have been investigated. It has been established that the most favorable conditions for growing optically and compositionally homogeneous heavily doped LiNbO₃ : Zn crystals, which are characterized by a low photorefractive effect, are implemented in the ZnO concentration range of ~4.0–6.76 mol % in the melt. Since the distribution coefficient K _eff decreases significantly with an increase in the ZnO concentration in the melt, one can obtain LiNbO₃ : Zn crystals with significantly different defect structures but identical zinc concentrations. A change in the zinc concentration in crystals has been shown to induce a stepwise change in the sequence order of the main (Li and Nb) and doping (Zn) cations and vacancies and stepwise anisotropic expansion of the oxygen octahedra along the polar axis. The number of kinks in the concentration behavior of the spectral-line widths (five kinks for the lines with frequencies of 630 (A ₁(TO)) and 876 cm^–1 (A ₁(LO))) significantly exceeds the number of thresholds (two) known from the literature.     

Structure and nonvolatile holographic recording of Mg:Ce:Cu:LiNbO3 crystals

A series of Mg:Ce:Cu:LiNbO₃ crystals has been grown by Czochralski method. Their infrared transmittance spectra and ultraviolet-visible absorption spectra were measured and discussed to investigate their defect structure. The nonvolatile holographic recording of Mg:Ce:Cu:LiNbO₃ crystals was characterized by the two-photon fixed method. We found that the recording time of Mg:Ce:Cu:LiNbO₃ crystals became shorter and nonvolatile diffraction efficiency decreases with the increase of Mg doping concentration, especially doping with Mg approaches and exceeds the so-called threshold. And the nonvolatility vanishes when the concentration of MgO exceeds 4 mol%. The intrinsic and extrinsic defects were discussed to explain the nonvolatile holographic properties in the Mg:Ce:Cu:LiNbO₃ crystals.     

Light scattering in single crystals of nonlinear-optical photorefractive LiNbO<Subscript>3</Subscript>:Cu and LiNbO<Subscript>3</Subscript>:Zn

Comparative studies are made of the photorefractive scattering of light in nonlinear single crystals of lithium niobate with congruent compositions (LiNbO₃) doped with "photorefractive" Cu [0.015 mass %] and "nonphotorefractive" Zn [0.5 mass %] cations. For the first time it is found that single crystals doped with "photorefractive" and "nonphotorefractive" cations have different indicatrices for photorefractive light scattering. The aperture angle for photorefractive scattering reaches its steady state value more rapidly with high laser powers than with low. However, at high powers laser induced heating of the crystal is greater, and this leads to a narrowing of the scattering indicatrix. It is also found that photorefractive scattering in these single crystals depends on the region of the boule from which a sample has been cut. This indicates that there is a nonuniform distribution over the boule of the imperfections with localized electrons which determine the magnitude of the photorefractive effect.     

Properties of thermally fixed holograms in photorefractive LiNbO<Subscript>3</Subscript>:Zn:Fe crystals

We have investigated the properties of thermally fixed holograms in LiNbO₃ crystals doped with the optical damage inhibitor Zn as well as the photorefractive Fe dopants. Time decays of fixed holograms at different temperatures showed a single thermally activated process with an activation energy of ∼1.08 eV. We have also studied the effect of an external electric field on the diffraction efficiency of these holograms. Results analysis has provided a new method to determine the photovoltaic field of the samples as well as the effective concentration of photorefractive traps.     

Formation dynamics of nonvolatile crossed-beam photorefractive gratings in doubly doped LiNbO3 crystals: Theoretical investigation

The formation dynamics of crossed-beam photorefractive gratings formed by the method of two-center holographic recording in doubly doped LiNbO₃ crystals is investigated in this paper based on the theoretical model combining the two-center band transport model with the two-dimensional coupled-wave theory. The numerical simulations are presented for two-center holographic recording crossed-beam photorefractive gratings in LiNbO₃:Fe:Mn crystals. The temporal and spatial evolutions of the refractive index modulation and the diffraction efficiency are shown. The spatial variation of the wave intensity is also presented.     

Effect of proton exchange and annealing on diffraction efficiency of Fe:LiNbO3 crystals

Influence of proton exchange and annealing on the photorefractive properties of Fe:LiNbO₃ crystals has been investigated using two-wave coupling phenomena. The two-wave coupling phenomena results in microscopic interference pattern inside the sample which subsequently helps in the formation of refractive index grating. The diffraction efficiency of the crystal increases after proton exchange, whereas the reverse is observed on annealed samples. The former is attributed to an increase of extraordinary refractive index of the crystal, while the latter to the oxidization of Fe²⁺ to Fe³⁺.     

高掺镁铌酸锂晶体的生长和倍频性能

我们通过测定MgO在同成分LiNbO₃中的有效分凝系数、相位匹配温度与MgO浓度之间的关系,找到了使Mg:LiNbO₃晶体的相位匹配温度达到最高的掺MgO配方,并克服了Mg:LiNbO₃晶体在高掺杂生长时易出现生长条纹和脱溶等问题,从而生长出了抗光折变能力强,光学均匀性良好的Mg:LiNbO₃晶体。用于连续泵浦Nd:YAG声-光调Q腔内倍频时,获得了平均功率最高达2瓦的二次谐波输出。 关键词：     

Grating formation in Fe:LiNbO<Subscript>3</Subscript> photorefractive crystal by chirped 800-nm femtosecond laser pulses operated at 1 kHz

We demonstrate an extension of forming a photorefractive volume grating in an Fe:LiNbO₃ crystal by chirped intense femtosecond laser pulses generated from a Ti:Al₂O₃ regenerative amplifier at 1 kHz. We confirm that one-photon absorption is still dominant in the Fe:LiNbO₃ crystal up to 70 GW/cm². To generate a photorefractive grating at such a low laser repetition rate within a practical writing time, the laser pulse intensity is increased to >30 GW/cm². Furthermore, we demonstrate the amplification of femtosecond laser pulses by the chirped volume grating that is written in the Fe:LiNbO₃ by two-wave mixing.