Ferroelectric domain inversion in near-stoichiometric lithium niobate for high efficiency blue light generation

LiNbO₃ single crystals with a composition close to stoichiometry ([Li]/[Li+Nb]=0.496), 16 mm in diameter and 40 mm in length were grown by the Czochralski method using K₂O flux. The domain reversal characteristics of near-stoichiometric LiNbO₃ single crystals were investigated. The switching field required for 180° ferroelectric domain reversal in the near-stoichiometric crystal at room temperature was 7.5 KV/mm. This is about one third of the switching field required for conventional LiNbO₃ crystals. Domain reversal (180°) in near-stoichiometric LiNbO₃ samples of 1.0 mm thickness has been achieved. Samples have been evaluated by second harmonic generation and conversion efficiencies of up to 32% have been obtained. Received: 8 November 2000 / Accepted: 29 January 2001 / Published online: 20 June 2001     

Role of stoichiometric point defect in electric-field-poling lithium niobate

Non-congruent LiNbO₃ crystals has been used to determine the influence of the intrinsic defect density in the ferroelectric domain inversion mechanism. The poling processes have been carried out either at high temperature or at RT throughout the electric-field-poling technique. It is shown that the coercive field of LiNbO₃ crystals is strongly influenced by the intrinsic defect density in the crystals. Moreover it is shown that it is possible to realign the ferroelectric domain structure of near-stoichiometric LiNbO₃ crystals to prepare periodic poled structures which allows second harmonic generation at shorter wavelengths than with congruent crystals at a fixed wavelength. Received: 6 July 1999 / Accepted: 24 November 1999 / Published online: 24 March 2000     

Defect structure and optical damage resistance of Hf:Fe:LiNbO3 crystals

A series of Hf:Fe:LiNbO₃ crystals were grown by the Czochralski technique with various doping concentrations of HfO₂. Their defect structures were analyzed by the UV-visible absorption spectra and infrared absorption spectra. The optical damage resistance of Hf:Fe:LiNbO₃ crystals was measured by the photo-induced birefringence change and the transmitted light spot distortion method. The results show that the optical damage resistance ability of Hf:Fe:LiNbO₃ crystals enhances remarkably with the HfO₂ concentration increasing when the HfO₂ concentration is lower than its threshold concentration (4 mol%). However, when the HfO₂ concentration exceeds its threshold concentration, the optical damage resistance ability of the crystals returns to decrease. This unusual behavior is explained by using the photovoltaic field produced in the crystals.     

Anomalous increase in the unipolarity of doped lithium niobate crystals in the temperature range 300–400 K

The lithium niobate single crystals doped with B, Zn, and Gd at a content of 0.002–0.44 wt % have been grown. Their domain structure, static and dynamic piezoelectric properties, dielectric properties, and conductivity are investigated over a wide range of frequencies. The dielectric dispersion associated with the Debye-type relaxation process and considerable anomalies in ?′₂₂(T) and conductivity are revealed in the temperature range ～300–400 K. At these temperatures, the piezoelectric modulus d ₃₃ of the initial polydomain crystals LiNbO₃: Gd jumpwise increases up to the values close to those for the undoped single-domain crystal. This increase is accompanied by a substantial change in the etch patterns due to the domain structure of the crystal. The nature of the anomalies observed in LiNbO₃ in the above temperature range is discussed.     

掺锌LiNbO3晶体的生长及其光学性能

在LiNbO₃中掺进3mol%、5mol%、7mol%ZnO生长Zn:LiNbO₃晶体.测试Zn:LiNbO₃晶体的吸收光谱,研究Zn:LiNbO₃晶体吸收边紫移的机制.测试Zn:LiNbO₃晶体的红外光谱,研究Zn(7mol%):LiNbO₃晶体OH 吸收峰由3484cm^-1移到3530cm^-1的机制.测试Zn:LiNbO₃晶体倍频转换效率和相位匹配温度,研究Zn:LiNbO₃晶体倍频转换效率增强的机制.     

Properties study of LiNbO3 lateral field excited device working on thickness extension mode

This paper investigates the properties of thickness extension mode excited by lateral electric field on LiNbO3 by using the extended Christoffel-Bechmann method. It finds that the lateral field excitation coupling factor for amode (quasi-extensional mode) reaches its maximum value of 28% on X-cut LiNbO3. The characteristics of a lateral field excitation device made of X-cut LiNbO3 have been investigated and the lateral field excitation device is used for the design of a high frequency ultrasonic transducer. The time and frequency domain pulse/echo response of the LiNbO3 lateral field excitation ultrasonic transducer is analysed with the modified Krimholtz-Leedom-Matthae model and tested using traditional pulse/echo method. A LiNbO3 lateral field excitation ultrasonic transducer with the centre frequency of 33.44 MHz and the -6 dB bandwidth of 33.8% is acquired, which is in good agreement with the results of the Krimholtz-Leedom-Matthae model. Further analysis suggests that the LiNbO3 lateral field excitation device has great potential in the design of broadband high frequency ultrasonic transducers.     

Nonvolatile photorefractive holographic recording in Sc:Ce:Cu:LiNbO3

In this paper experimental studies of nonvolatile photorefractive holographic recording in Ce:Cu:LiNbO₃ crystals doped with Sc(0,1,2,3 mol%) were carried out. The Sc:Ce:Cu:LiNbO₃ crystals were grown by the Czochralski method and oxidized in Nb₂O₅ powders. The nonvolatile holographic recording in Sc:Ce:Cu:LiNbO₃ crystals was realized by the two-photon fixed method. We found that the recording time of Sc:Ce:Cu:LiNbO₃ crystal became shorter with the increase of Sc doping concentration, especially doping with Sc(3 mol%), which exceeds the so-called threshold, and there was little loss of nonvolatile diffraction efficiencies between Sc(3 mol%):Ce:Cu:LiNbO₃ and Ce:Cu:LiNbO₃ crystals.     

Preparation and holographic storage properties of tri-doped Mg:Mn:Fe:LiNbO3 crystals

Doping MgO, MnO and Fe₂O₃ in LiNbO₃ crystals, tri-doped Mg:Mn:Fe:LiNbO₃ single crystals were prepared by the conventional Czochralski method. The UV-vis absorption spectra were measured and the shift mechanism of absorption edge was also investigated in this paper. In Mg:Mn:Fe:LiNbO₃ crystal, Mn and Fe locate at the deep level and the shallow level, respectively. The two-photon holographic storage is realized in Mg:Mn:Fe:LiNbO₃ crystals by using He-Ne laser as the light source and ultraviolet as the gating light. The results indicated that the recording time can be significantly reduced for introducing Mg²⁺ in the Mg:Mn:Fe:LiNbO₃ crystal.     

Spectroscopic analysis of Er transition in Mg/Er-codoped LiNbO3 crystal

We present a Judd-Ofelt spectroscopic analysis on the Mg/Er-codoped congruent lithium niobate (LiNbO₃) crystals. The Judd-Ofelt model is applied to the room temperature unpolarized absorption intensities of Er³⁺ ions on eleven transition bands to determine their intensity parameters: Ω₂=2.36×10⁻²⁰ cm², Ω₄=0.76×10⁻²⁰ cm², Ω₆=0.30×10⁻²⁰ cm² in Er:LiNbO₃ crystal heavily codoped with MgO. The radiative lifetime of ²H_9/2 becomes longer when MgO is added into Er:LiNbO₃ crystal. The experimental lifetimes are obtained using microsecond time-resolved spectra at 400 nm femtosecond pulse excitation to predict radiative quantum efficiency. Combining higher radiative quantum efficiency with longer radiative lifetime, we conclude that Mg/Er-codoped LiNbO₃ crystals are more suitable than Er: LiNbO₃ ones in laser materials.     

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     

Periodic domain structures formed under electron-beam irradiation in LiNbO3 plates and Ti:LiNbO3 planar waveguides of the Y cut

Regular domain structures on the Y cuts of the LiNbO₃ substrates and Ti:LiNbO₃ waveguide structures based on these substrates have been fabricated under electron-beam irradiation. It has been revealed that the domains in undoped and titanium-doped LiNbO₃ crystals are formed as a result of different processes. It has been demonstrated using chemical etching and waveguide second-harmonic generation that regular domain structures in the Ti:LiNbO₃ waveguides are formed at a depth of approximately 8 μm from the surface, where the titanium concentration does not exceed 2 mol %. The quasi-synchronous waveguide optical second harmonic generation with an efficiency of 8.8% has been obtained using the fabricated structures.     

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     

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.     

Measurement of Wavelength Dependence of Electro-Optic Coefficients r22 of Non-doped and 5% MgO-doped Congruent LiNbO3 Crystals and 1.8% MgO-doped Quasi-stoichiometric LiNbO3 Crystal by Multiple Reflection Interference Method

The electro-optic coefficient r ₂₂ in the wavelength range from 409 to 1580 nm was measured for non-doped and 5% MgO-doped congruent LiNbO₃ crystals and 1.8% MgO-doped quasi-stoichiometric LiNbO₃ crystals in a simple optical system using a multiple reflection interference method capable of producing high-precision results without the application of antireflection film to the end faces of the crystal. The influence of the manufacturing errors of the electrooptic crystals was discussed on the measurement of the r ₂₂ coefficient. The experimental errors are less than approximately 0.5% in the wavelength range from 409 to 1064 nm and approximately 1% from 1340 to 1580 nm. It was further shown that polarizing of the laser along X axis resulted in highly accurate measurement of the r ₂₂ of LiNbO₃ crystals.     

周期极化掺镁不同组分LiNbO3晶体的研究

利用气相平衡扩散法研制出掺镁不同组分的LiNbO₃晶体，并对其极化特性进行了研究.研究表明晶体的开关电场和自发极化不仅与晶体组分［Li］/［Nb］比有关而且与掺镁量有关，［Li］/［Nb］比为0.973掺入2mol% MgO的近化学比LiNbO₃晶体的开关电场仅为1.8kV/mm，是同成分晶体的1/12，且其极化结构的质量要远好于同成分LiNbO₃晶体和近化学比LiNbO₃晶体. 关键词： 气相平衡扩散 3晶体')" href="#">掺镁LiNbO₃晶体 周期极化     

Electroluminescence in lead titanate single crystals

Electroluminescence in PbTiO₃ single crystals is studied with variation in applied electric field, frequency (20 Hz to 5 kHz) and temperature. The EL onset depends on the rate at which the dipole switches. Extremely sharp upward rising nature of the pulses of micro second duration suggest that there is a self maintained discharge in the dielectric due to secondaryγ _p mechanism. Frequency dependence of EL suggests that both the secondary mechanisms, viz. theγ _p andγ _i are active after the application of a high field and the critical field at which this occurs decreases with increase in the frequency of the applied voltage. Similarly the onset voltage decreases with increase in frequency. The temperature dependence of EL at the applied frequency of 50 Hz shows that the onset voltage is intimately connected with the coercive field of the crystal and it is minimum at the Curie point. The study suggests that EL occurs in the bulk and there is a breakdown in the dielectric due to an avalanche formation.     

Raman study on vapor-phase equilibrated Er:LiNbO3 and Er:Ti:LiNbO3 crystals

Raman spectra of Er:LiNbO₃ crystal and Ti-diffusedEr:LiNbO₃ strip waveguide, in which the Li/Nb ratio was altered using a vapor-phase equilibration (VPE) technique, were measured at room temperature in the wave-number range 50–3500 cm^-1. Both 488 and 514.5 nm radiations were used to excite Raman scattering, A₁(TO) and E(TO) modes were recorded at backward scattering geometry. The results indicated that the lattice vibrational spectra of the as-grown Er:LiNbO₃ are almost the same as those of pure LiNbO₃ except for the little shift of the peak position and the change of relative intensity of some peaks. In comparison with the spectra of as-grown Er:LiNbO₃ crystal the vapor-phase equilibrated Er:LiNbO₃ and Er:Ti:LiNbO₃ crystals in the lattice vibrational region exhibit the following features: firstly, Raman peaks become narrow, indicating that the VPE process has brought Er:LiNbO₃ and Er:Ti:LiNbO₃ crystals closer to a stoichiometric composition; secondly, relative intensity of some peaks varies with the VPE time; and finally, slight blue shifting in peak position was observed. Some of these features were correlated with the NbO₆ octahedra and with the site distribution of the doped Er ions. In addition, green fluorescence peaks and/or bands associated with the electron transitions ² H _11/2?⁴ I _15/2 and ⁴ S _3/2?⁴ I _15/2 of the doped Er³⁺ were also observed. For 488 nm excitation they appear in the wavenumber range of 1200–3000 cm^-1 and are well separated from lattice vibrational region; for 514.5 nm excitation, however, these fluorescence peaks shift towards the low wavenumber region and overlap partially with the lattice vibrational spectra. Received: 24 May 2000 / Accepted: 29 May 2000 / Published online: 13 September 2000     

Mg2+对Fe:LiNbO3晶体光折变响应时间的影响

在Fe:LiNbO₃中掺进3mol%和6mol%MgO,生长了Mg:Fe:LiNbO₃晶体.测试了Mg:Fe:LiNbO₃晶体抗光致散射能力、衍射效率、响应时间和光电导.推导响应时间与光电导之间的关系.在Fe:LiNbO₃晶体中掺进6mol%的Mg²⁺,它的抗光致散射能力比Fe:LiNbO₃晶体提高一个数量级,响应速度比Fe:LiNbO₃晶体提高四倍.     

Comparison of two-color holography among different doped LiNbO3 crystals at low intensities

The effects of material and experimental parameters on the nonvolatile two-color holographic recording space charge field and sensitivity for different doped LiNbO₃:Fe crystals have been studied theoretically based on a two-center model. When the direct electron transfer between the deep-trap centers and the shallow-trap centers was considered, the near-stoichiometric LiNbO₃:Fe is confirmed theoretically to be of bigger space charge field and higher recording sensitivity than the LiNbO₃:Fe:Mn and LiNbO₃:Cu:Ce in the low intensity region. A further improvement of the recording sensitivity can be achieved by doping concentration, thermal reduction treatment of Fe, appropriate gating and recording wavelengths with large photo-excitation cross sections.     

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.