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ISSN 10637745, Crystallography Reports, 2012, Vol. 57, No. 7, pp. 909–911. © Pleiades Publishing, Inc., 2012. PHYSICAL PROPERTIES OF CRYSTALS Optical Parameters of Paratellurite Crystals A. I. Kolesnikova, I. A. Kaplunova, S. E. Il’yashenkob, V. Ya. Molchanovc, R. M. Grechishkina, M. A. Arkhipovaa, and S. A. Tret’yakova a Tver State University, Tver, 170002 Russia email: [email protected] b Tver State Technical University, Tver, 170026 Russia c National University of Science and Technology MISiS, Moscow, 119049 Russia Received December 20, 2010 Abstract—Refractive indices and transmittances of paratellurite single crystals have been measured. The spe cific optical rotation is determined and the Verdet constants are calculated for a radiation wavelength of 355 nm. DOI: 10.1134/S1063774512070115 INTRODUCTION Unique acoustooptic, nonlinear, and piezoelec tric properties of paratellurite (αTeO2) crystals make this material very promising for applications in many fields of science and technology. To date, the applica tion of paratellurite in devices using its optical proper ties has been limited by its intrinsic material absorp tion at a wavelength of 0.35 μm, which corresponds to the short UV range [1]. It was even believed that para tellurite crystals barely transmit 0.36μm light. Recently it was reported that, to a great extent, the weak light transmission at this wavelength is related, not to absorption, but to the sharp increase in reflec tance, which is in turn caused by the sharp increase in the refractive index [2]. It was also found that, in the range of 0.35–0.36 μm, there is a sharp increase in not only the refractive indices, but also in the specific optical rotation to values of more than 700 deg/mm [2], which are larger those predicted by the approximation depen dences obtained in the visible range [2–5]. The afore mentioned range includes a working wavelength of mod ern commercial lasers of 0.355 µm (the third harmonic of radiation of lasers with active media containing Nd3+ ions) [6]. Therefore, the optical properties of paratellu rite at this wavelength are of particular interest. MEASUREMENTS OF OPTICAL PARAMETERS OF PARATELLURITE CRYSTALS We measured the refractive indices of paratellurite crystals (αTeO2) for ordinary and extraordinary rays using an optical scheme that included a frequency doubled YAG:Nd3+ laser (λ = 355 nm), a digital cam era, a Laser Power Meter, and a large transparent sam ple with sizes of 60 × 45 × 40 mm along the [001], [110], and [ 110] axes, respectively, cut from a paratel lurite single crystal; all sample faces were polished. Since the laser partially emits the second harmonic with a wavelength of 533 nm, two beams were recorded at the output face for both ordinary and extraordinary rays: violet (UV induced fluorescence) and green. The distance between the centers of the corresponding spots on the crystal face, the angle of incidence, and the crystal thickness were used to calculate the No and Ne values. They were found to be No = 2.688 and Ne = 2.891, i.e., somewhat larger than those measured in [7] (No = 2.568 and Ne = 2.778). This means that the effi ciency of paratelluritebased acoustooptic devices that operate at a wavelength of 355 nm should exceed the value expected based on the previous data by 31– 32% because the optical quality factor of material Ì2 is proportional to the sixth power of the refractive index. The transmittances T of polished cubes with sides of 1 cm cut from paratellurite crystals were measured by the directed transmission method in [8, 9]. The corresponding T values for the wavelength of 355 nm in the [001] and [110] directions were found to be 0.66, and 0.62. These values are 5–8% larger than those established previously in [4]. This circumstance expands the range of applications of paratellurite in deflectors, as well as in the acoustooptic devices of multispectral spectroscopy in the part of the UV range that is very important for medical diagnostics, biolog ical studies, and astrophysics. Another possible appli cation of paratellurite is the fabrication of polarization and birefringent prisms for light in this range. Exact data on the gyrotropy of material are also necessary for designing acoustooptic waveguides and calculating the frequency characteristics of acousto optic devices because the diffraction of light by ultra sonic waves depends on the polarization state of trans mitted light [10, 11]. It should be emphasized that inaccurate values of specific rotation lead to an error in determining the component G33 = ρλ / π N 03 of the gyration pseudoten sor, which is used to calculate the acoustooptic inter actions [11]. Experimental data on the specific rota tion were obtained for a limited number of wave 909 910 KOLESNIKOV et al. ρ, deg/mm 700 600 500 400 300 200 100 400 lengths. Therefore, the corresponding curves ρ(λ) plotted using approximations [3] may yield inaccurate values of G33, especially for the spectral ranges where ρ(λ) values were not measured. Specifically, this prob lem was encountered in [11], where attempts were made to calculate the parameters of a UV acousto optic deflector based on TeO2 designed for operation at a wavelength λ = 0.355 μm (the third harmonic of YAG:Nd3+ laser radiation. An analysis of the studies on the gyrotropy of para tellurite shows that the data on the specific rotations ρ(λ) were obtained by measuring the intensity of light transmitted through a polarizer, sample, and analyzer [2, 3, 12]. The desired rotation of plane of polarization caused by the gyrotropy of the material was compen sated for by the analyzer rotation that was necessary to make to recover the initial intensity value. The resulting error included the errors related to the measurements of light intensities and angles. In addition, because of very large ρ(λ) values, especially in the spectral range of 0.35–0.5 μm (which is close to the fundamental absorption edge), the samples must have fairly small thickness of less than 1 mm. If not, the rotation of plane of polarization could be multiple. These diffi culties were noted in [3], where circular dichroism was λ, nm ρ(λ), deg/mm [14] ρ(λ), deg/mm 633 531 488 438 87 143 184 271 84.7 ± 0.3 146.0 ± 0.3 186.3 ± 0.3 600 700 λ, nm Fig. 2. Dependences ρ(λ), plotted according to data of [14] and this study. Fig. 1. Manifestation of gyrotropy and its dispersion at scattering of laser beams with different wavelengths, prop agating in a paratellurite single crystal 41.0 mm thick along the [001] optical axis: (upper) red beam, λ = 633 nm; (medium) green beam, λ = 533 nm; and (lower) blue beam, λ = 488 nm. Values of specific optical rotation in paratellurite crystals 500 measured: along with circular dichroism bands, oscil lations in the form sin(2ρl) (l is the sample thickness) were recorded, and it was necessary to use a special method to eliminate them. This led to additional errors caused by the errors in measuring the sample thickness and errors in the orientation of the sample. In this study, we measured the optical rotation on a paratellurite single crystal with sizes of 41.0 × 20.1 × 20.0 mm along the [001], [110], and [1 10] directions, respectively. All sample faces were polished. In the first stage, measurements were performed at laser wave lengths of 633, 533, and 488 nm, according to the technique described in [13]. Figure 1 shows patterns of laser beam scattering in paratellurite, which were used to determine the spe cific rotation by the aforementioned method. The cal culated values of specific rotation ρ(λ) and the values found in [14] are listed in the table. These data were used to perform approximations in which the best cor relation coefficients were obtained with the function (1) ρ −1 = a + bλ 2 ln ( λ), where λ and ρ(λ) are measured in angstroms and deg/mm, respectively. The corresponding coefficients were found to be a = –0.00283 and b = 4.06 × 10–11. The table contains the comparative values of specific rotation, which were determined experimentally in this study and in [14]. As follows from the table, at large (small) wave lengths, the known values [14] of specific optical rota tion are larger (smaller) than those found in this study. Figure 2 shows the dependences ρ(λ), which were plotted by approximating the values obtained in [14] and in this study. In the latter case, the best approxi mation is given by the formula ρ −1 = a + bλ 2 ln ( λ), where a = –0.00310 and b = 4.17 × 10–11. CRYSTALLOGRAPHY REPORTS Vol. 57 No. 7 (2) 2012 OPTICAL PARAMETERS OF PARATELLURITE CRYSTALS According to both dependences, the specific rota tion for a wavelength of 355 nm should not exceed 750–800 deg/mm. However, direct measurements of the rotation of the plane of polarization of the UV beam in the sample (Fig. 1) after its thinning by 40 μm and repolishing yielded another value of 840 ± 8 deg/mm. Thus, the value of the gyration pseudotensor G33 in paratellurite at 355 nm was also larger than previously expected. Then, we measured the Faraday rotation in paratel lurite for a wavelength of 355 nm. The Faraday effect implies the rotation of the plane of polarization of a beam that propagates coaxially with the vector H of a dc magnetic field applied to the crystal. The rotation of plane of polarization by an angle θ is related to the crystal length l in the field direction by the relation [13] (3) θ = VHl , where V is the Verdet constant. The following V values were obtained in [5] for two radiation wavelengths: V(λ = 533 nm) = 6.11 × 10–5 rad A–1 and V (λ = 633 nm) = 3.78 × 10–5 rad A–1. In this study the Verdet constant was measured for UV laser radiation with a wavelength λ = 355 nm. To measure the Faraday rota tion, we cut a cubic sample from a paratellurite single crystal; this cube had sizes of 1 × 1 × 1 cm along the [001], [110], and [ 1 10 ] axes, respectively, and pol ished (001) faces. The cube was placed between the polarizer and analyzer so as to orient the laser beam be perpendicularly to the input (001) face and make it pass through the face center. A photodetector (Laser Power Meter) was placed behind the analyzer; the photodetector signal was amplified and applied to the measurement scheme. An annular permanent Nd–Fe–B magnet with an inner diameter of 2.0 cm was used to generate a dc magnetic field. The magnetic field strength on the magnet axis was 1.43 × 105 A m–1. The magnet could be moved along the optical scheme and coaxially approach the crystal. First, in the absence of a magnet, the laser beam was suppressed by the analyzer to minimum. Then, the magnet was moved toward the crystal. The rotation of plane of polarization was detected by an increase in the photo current. Then, the beam outgoing from the crystal was suppressed again to minimum by rotating the ana lyzer; the latter was equipped with an angle counter (having an error of ±0.5′). The angle of rotation of the plane of polarization θ was found to be 14°40′ ± 0.5′. According to (3), this yields the Verdet constant V = 1.7 × 10–4 rad A–1 for the wavelength λ = 355 nm. The dispersion of the Faraday effect is approximately described by the formula [13] (4) V = A λ2 + B λ4 . The dispersion constants were calculated in [1]: A = 3.37 × 10–14 m2 rad A–1 and B = 2.06 × 10–30 m4 rad A–1. According to these values, the angle of rotation of plane of polarization under the conditions of our experiment should not exceed 12°. Thus, paratellurite exhibits CRYSTALLOGRAPHY REPORTS Vol. 57 No. 7 911 also a sharp enhancement of magnetooptical proper ties near the fundamental absorption edge. In princi ple, the large value of the Verdet constant can be used to design paratellurite modulators of 355nm laser radiation, whose operation is based on the Faraday effect rather than on acoustooptic interactions. CONCLUSIONS The values of the refractive indices, transmittances, specific optical rotation, and Verdet constants mea sured in paratellurite single crystals for 355nm light turned out to be larger than the previously published values. This circumstance presents new prospects for the application of paratellurite as a material for acoustooptic waveguides in acoustooptic deflectors and acoustooptic filters for a multispectral analysis of microscopic and telescopic images, as well as for bire fringent prisms and magnetooptical modulators operating in the UV range. ACKNOWLEDGMENTS This study was supported by the Federal Target Program “Scientific and ScientificPedagogical Per sonnel of Innovative Russia” for 2009–2013. REFERENCES 1. A. I. Kolesnikov, R. M. Grechishkin, V. Ya. 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Molchanov, Acoustooptic Devices and Their Applications (Gordon and Breach, New York, 1989). 11. V. Ya. Molchanov, O. Yu. Makarov, A. I. Kolesnikov, and Yu. M. Smirnov, Vestn. TvGU, Ser. Fiz., No. 4(6), 88–93 (2004). 12. N. Uchida, Phys. Rev. B 4 (10), 3736 (1971). 13. V. Yu. Vorontsova, R. M. Grechishkin, I. A. Kaplunov, et al., Opt. Spektrosk. 104 (5), 822 (2008). 14. A. Yariv and P. Yeh, Optical Waves in Crystals: Propaga tion and Control of Laser Radiation (Wiley, New York, 1984; Mir, Moscow, 1987). 2012 Translated by Yu. Sin’kov