LiNbO3:Cu:Ce晶体非挥发全息存储性能的理论研究

以双中心模型为基础, 理论研究了LiNbO₃:Cu:Ce晶体在稳态情况下的非挥发双光双步全息存储性能. 研究中考虑了在晶体深能级中心Cu⁺/Cu²⁺ 与浅能级中心Ce³⁺/Ce⁴⁺ 之间由隧穿效应引起的电荷直接交换过程. 结果表明, 总的空间电荷场大小主要由深能级上的空间电荷场所决定, 并且非挥发全息存储性能主要由隧穿效应引起的深能级中心Cu⁺/Cu²⁺ 与浅能级中心Ce³⁺/Ce⁴⁺ 之间的电荷直接交换过程所决定. 与隧穿效应相关的材料参数对于非挥发双光双步全息存储的性能起到了至关重要的作用.     

Fast electrically switchable holographic optical elements in LiNbO3

We present here the realization of fast electrically switchable holographic optical elements based on electric field multiplexing of volume holograms in lithium niobate crystals. We demonstrate the electrical control of holographic lenses and holographic mirrors for fast switching of the focal length and the direction of the reconstructed light beam, respectively. The switching time in the range of few hundred microseconds has been demonstrated using this technique.     

Intensity dependence of two-center nonvolatile holographic recording in LiNbO3:Cu:Ce crystals

Nonvolatile photorefractive gratings have been recorded in LiNbO₃:Cu:Ce crystals by using a He–Ne laser (633 nm) for recording and an argon ion laser (458 nm) for sensitizing. The sensitizing light increases the recording sensitivity by a−bexp(−I_s/c) and saturation behavior will appear with high enough intensity of sensitizing light. The recording light increases the slope of η^1/2 as a function of time during the initial stages of hologram formation by sublinear I^x_r (x<1) and thus the recording light decreases the recording sensitivity. The dependence of saturation diffraction efficiency on the intensities of the recording and sensitizing light shows that there is a maximum dynamic range of the recording process.     

Oscillation of nonvolatile holographic recording in LiNbO3:Fe:Cu crystals

The oscillation of diffraction efficiency is observed in the nonvolatile holographic recording of lithium niobate crystals doped with iron and copper. The physics of oscillation in doubly doped lithium niobate crystals is studied by using Runge–Kutta methods, and the oscillation can be attributed to the redistribution of electrons in the deeper and shallower traps of the crystals in the initial phase of holographic recording. The effects of Fe concentration and intensity ratio of red beams to UV beam (I_R/I_UV) on the oscillation are investigated theoretically. The results show that with lower Fe concentration, the amplitude of oscillation is larger and with lower intensity ratio I_R/I_UV, the duration of the oscillation is longer.     

Nonvolatile hologram storage properties of tri-doped Zn:Ce:Cu:LiNbO3 crystals

Congruent Zn(7 mol%):Ce:Cu:LiNbO₃ single crystal was grown by the Czochralski method in air. The occupation mechanism of the Zn²⁺ was discussed by an infrared transmittance spectrum. The nonvolatile holographic recording in Zn(7 mol%):Ce:Cu:LiNbO₃ single crystal was measured by two-photon fixed method. Zn(7 mol%):Ce:Cu:LiNbO₃ single crystals present the faster recording time and higher light-induced scattering resistance ability comparing with Ce:Cu:LiNbO₃ single crystals.     

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.     

Application of interference microscopy to the study of hologram build-up in LiNbO3 crystals

Interference microscopy was applied to direct microscopic observation of temporal evolution of phase holograms in LiNbO₃:Fe photorefractive crystals. First a hologram was recorded in the sample, and diffraction efficiency was monitored during hologram build-up using inactinic laser light. Thus kinetics of hologram build-up could be determined. The initial hologram was erased using white light. Then a series of write-erase cycles were performed with increasing exposure times. Holograms were observed by interference microscope after each exposure. The time elapsed between the exposure and the microscopic observation was negligible compared to the relaxation time of the hologram. The obtained temporal evolution of the grating profile gives a deeper insight into the physical mechanism of hologram formation in photorefractive materials than simple diffraction efficiency measurements. A congruently grown sample of LiNbO₃ doped with 10⁻³ mol/mol Fe in melting was studied by this method. Sample thickness was set to 300 μm to allow correct microscopic observation. Plane-wave holograms were recorded in the samples using an Ar-ion laser at λ = 488.0 nm of grating constants of 3, 6.5 and 8.8 μm.     

Space charge field limitations in photorefractive LiNbO3:Fe crystals

We use holographic techniques for the investigation of strongly oxidized LiNbO₃:Fe crystals with small Fe²⁺ concentrations and compare the results with theoretical predictions. Experimental evidence is presented for enhanced phase shifts between light intensity pattern and refractive index grating and for limitations of optically induced space charge fields in photovoltaic crystals due to the low concentration of filled traps. Our findings do not support the model of a nonlocal photovoltaic effect in LiNbO₃.     

Holographic angle multiplexing combined with peristrophic multiplexing in a photorefractive LiNbO3 crystal

We have investigated angle multiplexing combined with peristrophic (rotational) multiplexing in a photorefractive LiNbO₃ crystal of cylindrical shape. The peristrophic multiplexing was achieved by rotating the recording medium while the angle multiplexing, by varying the incident angle of the reference beam. Angle multiplexing in synchronization with rotation of the sample made it possible to continuously record and retrieve holograms. In the combined multiplexing, holograms were stored at different peristrophic positions and thus their angular selectivity could be much improved in comparison to that of only angle-multiplexed holograms. The theoretical angular selectivity was derived, along with its dependence on the sample rotation. The experimentally measured selectivity was in agreement with the theoretical one. The angular selectivity of angle-multiplexed holograms was measured to be 0.03° in the absence of sample rotation and it became less than 0.0075° with a sample rotation by 5.4°.     

Incoherent one beam recording in LiNbO3

We find a way to record and retrieve images in a photorefractive LiNbO₃ crystal using a single white light source instead of a coherent light source. According to the experimental results, we think this recording is not due to the recording of fanning gratings, but a variation of refractive index responding to the non-uniform illumination. We have also simulated the recording using the band transport model taking into account the photovoltaic effect. The simulation result agrees with the experimental results.     

Growth and optical properties of In:Nd:LiNbO3 crystals

In, Nd double-doped LiNbO₃ (LN) crystals have been grown for the first time. Their infrared (IR) transmission spectra were measured and discussed to investigate their structure and defects. The optical damage resistance of Nd:In:LiNbO₃ crystals were characterized by straightly observing transmission facula distortion method. The optical damage resistance of In (4.0 mol%):Nd:LiNbO₃ was much higher than that of Nd:LiNbO₃. The defects were discussed in this paper to explain the optical damage resistance in the In:Nd:LiNbO₃ crystals.     

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⁺.     

Investigation of nonvolatile holographic storage in LiNbO3:Mn:Ce:Fe crystal

We investigate the persistent holographic recording in triply doped LiNbO₃:Mn:Ce:Fe crystals at different oxidation/reduction states. The experimental results show that there is an optimum oxidation/reduction state, which results in the best dynamic range M/#. Compared with doubly doped LiNbO₃:Ce:Fe, we found that the nonvolatile diffraction efficiency and the best dynamic range M/# obtained in triply doped samples are larger than that obtained in doubly doped samples. The reason for the increase of the crystal about the nonvolatile diffraction efficiency and the dynamic range M/# was also explained.     

Improved nonvolatile holographic storage sensitivity of near-stoichiometric LiNbO3:Fe:Mn crystals

We investigate the nonvolatile holographic storage characteristics of near-stoichiometric LiNbO3 :Fe:Mn crystals with different Li2O contents. Experimental results indicate that the optimal value of Li2O content is about 49.6 mol%. Nonvolatile sensitivity S considerably improved to 0.15 cm/J because of the use of near-stoichiometric LiNbO3 :Fe:Mn with 49.6 mol% Li2O.     

Study of near-infrared nonvolatile two-center holographic recording in LiNbO3:Fe:Rh crystal

The near-infrared nonvolatile holographic recording has been realized in a doubly doped LiNbO₃:Fe:Rh crystal by the traditional two-center holographic recording scheme, for the first time. The recording performance of this crystal has been investigated by recording with 633 nm red light, 752 nm red light and 799 nm near-infrared light and sensitizing with 405 nm purple light. The experimental results show that, co-doped with Fe and Rh, the near-infrared absorption and the photovoltaic coefficient of shallow trap Fe are enhanced in this LiNbO₃:Fe:Rh crystal, compared with other doubly doped LiNbO₃ crystals such as LiNbO₃:Fe:Mn. It is also found that the sensitizing light intensity affects the near-infrared recording sensitivity in a different way than two-center holographic recording with shorter wavelength, and the origin of experimental results is analyzed.     

OH-absorption properties of the optical damage region in codoped In/Mg:LiNbO3 crystals with various Li/Nb ratios

OH-absorption properties of the optical damage region in a series of codoped In/Mg:LiNbO₃ crystals with various Li/Nb ratios have been investigated. The OH⁻-associated vibrational peak at 3507 cm⁻¹ is confirmed to occur in crystals with Li/Nb ratio of 0.94. For codoped In/Mg:LiNbO₃ crystals with Li/Nb ratio of 1.05 and 1.20, the OH⁻-associated vibrational peaks are detected at 3536 and 3507 cm⁻¹ as well. A new peak at 3518 cm⁻¹ attributed to a (In_Nb)²⁻-OH⁻-(Mg_Nb)³⁻ defect center is revealed in crystals with Li/Nb ratio 1.38. When the “In-Mg threshold” concentration is reached, the optical damage resistance ability of codoped In/Mg:LiNbO₃ crystals is greatly improved.     

Infrared holographic recording in LiNbO3:Cu

Holograms may be recorded in photorefractive LiNbO₃:Cu with pulsed infrared light (wavelength =1064 nm, Q-switched Nd:YAG laser), if the crystals are previously or simultaneously illuminated with a green (=532 nm) light pulse. We study refractive index changes and time constants of as-grown and thermally treated crystals with different copper concentrations. A model explaining this effect is discussed.     

Experimental evidence of a non-relationship between photorefractive inhibition and photoconductivity increase in LiNbO3:Mg

By means of measurements of both photoconductivity and two-wave mixing using cw 532 nm laser light, a direct relationship between optical damage resistance and photoconductivity coefficient for several congruent magnesium-doped lithium niobate crystals, with concentrations below and above the threshold of around 4.6 mol% MgO in melt, has not been observed. Specifically, when the polar axis is parallel to the photorefractive grating vector formed by two-interference beams, an increase of optical-damage resistance above the threshold is obtained. However, the photoconductivity coefficient is of the same magnitude of those samples below the threshold. On the other hand, when the optical axis is perpendicular to the grating vector, a decrease of the refractive index grating for crystals below the threshold could be observed, but even for this case the photoconductivity coefficient is unchanged, except for only one specimen with high magnesium level which exhibits simultaneously photorefractive response and high photoconductivity. These results suggest that the increase of photoconductivity is not very essential in the process of photorefractive inhibition; rather, the distribution of magnesium ions with respect to polar axis is an important parameter in the mechanism of optical-damage resistance.     

High-sensitivity read-write volume holographic storage in reduced KNbO3 crystals

Reduced KNbO₃ is a photoconductive ferroelectric in which holograms can be recorded by the photorefractive effect. Read-write volume hologram storage and erase sensitivities ofS ⁻¹=100 J/cm² andS ⁻¹=84 J/cm² (S=d(Δn)/d(I₀t)‖_t=0) have been measured at zero applied electric field, where the charge transport is shown to be due to diffusion of photoexcited electrons. By applying an electric field along thec-axis, the migration length of the photoexcited electrons becomes comparable to the holographic grating spacing. This leads to storage sensitivities comparable to high-resolution photographic plates. Experimental data on storage and erase sensitivity as a function of the grating spacing, applied electric field, writing light intensity and temperature are reported and interpreted on the basis of the theoretical results of Young et al. and Amodei. Changes of the intensity ratio of the writing beams by self diffraction (beam coupling), reflections from surfaces and the residual dark conductivity are assumed to cause experimental results which deviate from the theoretical models. It is shown, that in reduced KNbO₃ and other ferroelectric photoconductors having photocarrier transport lengths much larger than the unit cell dimension, photovoltaic currents do not contribute significantly to the build-up of space-charges leading to the photorefractive effect.     

Emission characteristics of Er in vapor-transport-equilibrated Er/Zn-codoped LiNbO3 crystals

Polarized visible and infrared emission characteristics of Er³⁺ ions in vapor-transport-equilibration (VTE)-treated LiNbO₃ crystals codoped with different concentrations of Zn and Er were investigated in comparison with corresponding as-grown crystals. The results show that the VTE treatment leads to substantial spectral changes of Er³⁺ emissions at 0.65, 0.98 and 1.5 μm regions, and the spectral changes in the 0.98 and 1.5 μm regions appear to be Zn-concentration-dependent. It is concluded in combination with X-ray powder diffraction results and optical absorption characteristics reported previously that the VTE treatment resulted in crystalline phase transformation with respect to Er³⁺ ions from original LiNbO₃ to ErNbO₄ phase in all crystals studied. The formation of the ErNbO₄ phase and the Zn²⁺ codopants are responsible for the VTE-induced substantial spectral changes. The emission characteristics of the ErNbO₄ precipitates in the Zn/Er-codoped crystals are found to be very different from those of the ErNbO₄ precipitates in the only Er-doped crystal in the infrared region, and the difference is attributed to the influence of the Zn²⁺ codopant on the Er³⁺ ion environment. The mechanism of the crystalline phase transformation is qualitatively explained from the viewpoint of the declined solubility of Er³⁺ ion in a Li-rich LiNbO₃ crystal and from the phase diagram of Li₂O-Nb₂O₅ system.