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.     

Photorefractive light scattering in lithium niobate crystals doped with Mg2+, B3+, Y3+, and Ta5+

We have investigated the photorefractive (photoinduced) light scattering in lithium niobate single crystals: LiNbO₃, LiNbO₃:B, LiNbO₃:Y(0.46 mas %), LiNbO₃:Y(0.24):Mg(0.63 mas %), and LiNbO₃:Ta(1.13):Mg(0.0109 mas %) that were grown from congruent melts. We have found that the shape of the speckle structure of this scattering and the kinetics of the development of its indicatrix depend substantially on the type of the impurity dopant in the lithium niobate crystal. We have observed that, upon laser irradiation of crystals doped with Y³⁺, Ta⁵⁺:Mg²⁺, and Y³⁺:Mg²⁺, the shape of their scattering indicatrix changes with time. At the same time, the LiNbO₃:B crystal is characterized by a complete absence of time changes in its speckle structure, which indicates that the photorefractive effect in this crystal is substantially lowered.     

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.     

Annular structures in photorefractive light scattering in a LiNbO3:Fe crystal

Ring-shaped photoinduced light scattering in pure and iron-doped lithium niobate crystals is found and studied under irradiation by a laser beam directed perpendicularly to the optic axis of the crystal. The scattering is observed in the directions of both reflected and transmitted pump beams. The structure and kinetics of the reported photorefractive scattering suggest that the phase-matching condition should be fulfilled in the vector interaction of the pump and scattered beams.     

Raman spectra of photorefractive lithium niobate single crystals

We have conducted comparative studies of the Raman spectra of lithium niobate (LiNbO₃) crystals of different compositions for excitation in the visible and near IR regions. We have observed that the photorefractive effect is one of the factors leading to line broadening. For this reason, the linewidths may be greater upon Raman excitation in the visible region than for excitation in the near IR region. This may be explained by formation in the crystal, when illuminated by laser radiation in the visible region, of a three-dimensional sublattice of nanostructures and microstructures (with refractive index and other physical parameters different from the parameters of the host crystal) from which photorefractive light scattering occurs. Formation of nanostructures and microstructures makes an additional contribution (besides the contribution due to random and dynamic disorder in the arrangement of the structural units) to the broadening of the Raman lines in the visible region of the spectrum. Illumination of the crystal by radiation in the near IR region does not induce a sublattice of nanostructures and microstructures, due to a significantly smaller photorefractive effect.     

Photoinduced gratings in a Sn<Subscript>2</Subscript>P<Subscript>2</Subscript>S<Subscript>6</Subscript> ferroelectric crystal with the period depending on the optical pump power

The light scattering in the form of ring structures in Sn₂P₂S₆ crystals at the propagation of intense laser pump radiation along the b crystallographic axis is detected. Radiation passing through a crystal is completely scattered into a cone whose angle increases with the pump power and decreases reversibly with a decrease in this power. The observed effect can be attributed to a spontaneous increase in the amplitude of photoinduced bulk diffraction gratings and to the scattering of light on them in the directions where the phase increments of the photorefractive and diffraction natures compensate each other. A similar type of scattering was observed previously in other photorefractive crystals, but the appearance of gratings with the period easily varied by varying the pump power is demonstrated for the first time.     

Self-action of Bessel light beams in cubic gyrotropic photorefractive crystals

We have studied conversion and interaction of a Bessel laser beam of zero order in photorefractive crystals. We have established that in a cubic gyrotropic crystal, two Bessel light beams propagate with different wave vectors and cone angles, but with identical conicity parameters. As the power in the Bessel light beam increases, we have experimentally observed a new optical effect: self-action of a Bessel light beam. We have studied the effect of external influences and the parameters of the beam itself on the process of self-refraction in photorefractive crystals. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 73, No. 4, pp. 488–493, July–August, 2006.     

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.     

Influence of surroundings on photorefractive effect in lithium niobate crystals

In the paper results of the investigation of the influence of electric properties of the environment surrounding LiNbO₃ crystals on photorefractive effect induced in these crystals by Gaussian Ar⁺ laser beam with various intensities are presented. We show spatial and temporal dependences of changes of the refractive index obtained experimentally in LiNbO₃: Fe and LiNbO₃: Fe:Mn samples surrounded by media with different electric conductivities and different permittivities (water, air, water solution of CaCl₂). The space and time dependences of the refractive index changes induced by the Ar⁺ laser beam are observed by means of the Mach–Zehnder interferometer using light from HeNe laser. The experimentally obtained results are in a good agreement with those following from numerical calculations using the manifold mirroring method. The agreement between calculated and experimental results indicates that the polarization charge at the photorefractive crystal/surrounding medium boundary significantly influences the photorefractive process in the crystal. The experimentally observed slow spontaneous decrease of the refractive index change in a sample placed into a slightly conducting medium (air) after switching off the beam also indicates that the polarization charge in the sample's surroundings affects the photorefraction.     

Conical parametric scattering of a single extraordinary beam in BaTiO3 crystal

In this paper, the parametric scattering of a single extraordinary polarized beam of laser in BaTiO₃ photorefractive crystal has been investigated experimentally and theoretically. The resulting pattern consists of beam fanning, isotropic ring, and anisotropic one. Among all parts of scattering pattern, isotropic ring has not been studied as much as beam fanning and anisotropic ring, and there still are some differences in reports about it. Therefore, the study has mainly focused on this part. In this experimental configuration, isotropic ring is just visible in positive angles although the other parts of parametric scattering pattern can be visible from behind and in front of the crystal. In addition to steady state pattern in forward and backward directions, its transient behavior with the rotation of crystal has been studied. The results of experiments have been analyzed carefully, and their theoretical explanations have been presented based on the standard theory of parametric scattering in photorefractive crystals. It has been shown that this configuration corresponds to the so called parametric B-process scattering.     

Effect of rhodium doping on the photorefractive properties of BCT crystals at 850 nm

We present an experimental investigation of the photorefractive properties of rhodium-doped barium calcium titanate (BCT) crystals of the congruent melting composition Ba_0.77Ca_0.23TiO₃. Considering the results previously obtained on this crystal in the visible region, it should be a good alternative to BaTiO₃. Nevertheless, many applications use infrared light. Therefore we present here a study of rhodium-doped BCT crystals at 850 nm. This wavelength is of special interest as it is in the spectral range of laser diodes. Rhodium doping is expected to enhance the sensitivity of the crystal in the infrared as is the case for BaTiO₃.We first noticed that BCT:Rh crystals are sensitive at this wavelength as expected. Furthermore, the photorefractive properties are interesting in terms of photorefractive gain, with a gain as high as 3 cm^-1 with ordinary polarization. This study has also put forward the fact that rhodium is not the only defect that participates in the photorefractive effect. Indeed, a large quantity of iron seems to be present in the BCT crystals and to participate in the photorefractive effect.An Erratum to this article can be found at     

Photorefractive light scattering in LiNbO3: Cu crystals

The time dependence of the photorefractive light scattering in lithium niobate single crystals of the congruent composition (LiNbO₃) doped by “photorefractive” Cu cations (0.015 wt %) is studied for a radiation power of 160 mW. The data for the photorefractive scattering are confirmed by changes in Raman scattering spectra.     

Hanbury-Brown and Twiss type double-slit interference with photorefractive fanning light

This paper reports that when an intense extraordinary-polarized laser beam illuminates a photorefractive BaTiO₃ crystal, the dynamic beam fanning light is formed to be a thermal-like light source with a long correlation time and wide spectral bandwidth. The experimental results of the first- and second-order double-slit interference with such photorefractive fanning light source, can be understood with the theoretical simulation in terms of Hanbury-Brown and Twiss effect.     

Optical homogeneity,defects, and photorefractive properties of stoichiometric,congruent, and zinc-doped lithium niobate crystals

Using the laser-conoscopy method, the photorefractive light-scattering method, and the Raman light-scattering method, we have studied the structural and optical homogeneities and photorefractive properties of (i) stoichiometric lithium niobate crystals (LiNbO₃(stoich)), which were grown from a melt with 58.6 mol % of Li₂O; (ii) congruent crystals (LiNbO₃(congr)); and (iii) congruent crystals that were doped with Zn²⁺ cations (LiNbO₃:Zn; [Zn] = 0.03–1.59 mol %). We have shown that the speckle-structure of the photorefractive light scattering in all the crystals is three-layer. The shapes of the second and third layers repeat in general the shape of the first layer. We have shown that the differences that are observed between the Raman spectra, the photorefractive light scattering, and the conoscopic patterns of the examined crystals are caused by the fact that defects are distributed inhomogeneously over the volume of these crystals and that Zn²⁺ cations are incorporated inhomogeneously into the lattice. This leads to the appearance of local changes in the elastic characteristics of the crystal and to the appearance of mechanical stresses, which locally change the optical indicatrix and, correspondingly, the conoscopic pattern and the Raman spectrum.     

Effect of XeCl laser irradiation on the defect structure of Nd:YAG crystals

This paper presents the effect of XeCl laser irradiation on Nd:YAG single crystal samples with various number of pulses at different repetition rates and laser fluences. Effects of the irradiation on the optical and structural properties of the crystal are analyzed by UV–vis-NIR spectroscopy. Annihilation of some point defects of the crystal structure is observed following laser irradiation at a fluence of 100 mJ cm⁻² with 100 and 500 pulses. Increasing the laser fluence and pulse numbers leads to saturation and new defects are found to be formed in the crystal. Additional absorption spectra of the irradiated samples show that oxygen vacancies in the Nd:YAG crystals are removed during the low-dose irradiation. The laser irradiation is compared to the thermal annealing process for Nd:YAG crystal modification. Additional absorption spectrum of an annealed sample reveals that induced negative absorption band at 236 nm is correlated with the annihilation of the oxygen vacancy center. Our results also demonstrate that XeCl laser treatment has several advantages upon annealing at high temperatures in the Nd:YAG crystal quality improvement. Thus, the present work can give a new approach to modify Nd:YAG crystals to be used in a wide variety of solid-state laser engineering.     

Structural homogeneity of photorefractive LiNbO<Subscript>3</Subscript> crystals doped with 0.03–4.5 mol % of ZnO

Using the electronic spectroscopy method, the laser-conoscopy method, and the Raman light-scattering method, we have studied the structural homogeneity of LiNbO₃ crystals doped with 0.03–4.5 mol % of ZnO. We have found that, as the laser radiation power is increased to 90 mW, the conoscopic patterns of crystals show additional distortions, which are attributed to the manifestation of the photorefractive effect. For the LiNbO₃ crystal doped with 4.5 mol % of ZnO, in which the photorefractive effect is low, we have revealed a considerable shift (compared to the remaining crystals) of the optical absorption edge toward the shortwavelength range, which indicates a high structural homogeneity of this crystal. We have shown that, in the LiNbO₃ crystal doped by 0.05 mol % ZnO, due to the displacement of Nb_Li and Li□ structural defects by Zn²⁺ cations, the crystal structure is ordered and, simultaneously, the number of defects with localized electrons decreases.     

Linear and nonlinear propagation of light beams in two-dimensional photorefractive photonic lattices formed in lithium niobate

Special features of linear and nonlinear propagation of coherent light beams in two-dimensional photorefractive photonic lattices optically induced in the lithium niobate crystal doped with iron are experimentally investigated. The two-dimensional gratings are formed by consecutive recording of two one-dimensional photorefractive gratings in the crystal. Experiments were performed using He-Ne laser irradiation with a wavelength of 633 nm. __________ Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 9, pp. 58–62, September, 2006.     

光折变晶体LiNbO_3:Fe中的特殊散射现象

用柱面透镜把经针孔滤波器扩束的激光束沿某一个方向聚焦成细丝状(或长条状),细丝状光束垂直入射到LiNbO_3:Fe晶体上,在远场位置观察散射光.我们发现光散射的方向与晶体的c轴方向不一致,不仅沿着晶体的c轴方向有散射光出现,沿光束的条形方向也出现很强的散射光.     

Photorefractive and optical scattering properties of Zr:Fe:LiNbO3 crystals

The LiNbO₃ crystal co-doped with ZrO₄ and Fe₂O₃ has been grown with [Li]/[Nb]=0.85 and 1.20, respectively, by the Czochralski method in air atmosphere. The incident exposure energy flux threshold for the light-induced scattering was characterized to investigate the scattering properties of the crystals. Applying the results of the incident exposure energy flux threshold effect, the photorefractive properties at different laser wavelengths (473 nm and 532 nm) were also measured by using the typical two-wave coupling experiments. The results show that Zr:Fe:LiNbO₃ crystal has a larger refractive index change, higher recording sensitivity and larger two-wave coupling gain coefficient at 473 nm wavelength than those obtained at 532 nm wavelength under the same experimental conditions. Moreover, the photorefractive properties decrease with the increasing [Li]/[Nb] ratios. The material of Zr:Fe:LiNbO₃ crystal is a promising candidate for blue photorefractive holographic recording.     

低功率近红外光的偏振方向对光致折射率变化影响的实验研究

研究了利用低功率近红外光辐照In:Fe:LiNbO3晶体时写入光束的偏振方向对光致折射率变化(Δn)的影响.分别采用正常偏振(o光)和非常偏振(e光)的近红外细激光束,在In:Fe:LiNbO3晶体中进行了光折变实验.研究表明,两种偏振方向引起晶体的Δn实测曲线相似,但变化规律恰好相反,o光引起的折射率变化量约是e光的3倍左右.近红外光写入下两种偏振光束引起晶体的Δn分布规律都不同于可见光,尤其是e光辐照区域中心晶体的折射率升高.因此,通过选择不同偏振方向的近红外光可以在光折变晶体中制作不同折射率分布的非线性光学器件.