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∑ ∑ ∫ Short Range Order in Powder of Amorphous Anodic Yttrium Oxide

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∑ ∑ ∫ Short Range Order in Powder of Amorphous Anodic Yttrium Oxide Crystallography Reports, Vol. 48, No. 4, 2003, pp. 531–535. Translated from Kristallografiya, Vol. 48, No. 4, 2003, pp. 583–587. Original Russian Text Copyright © 2003 by Aleshina, Loginova. CRYSTAL CHEMISTRY Short Range Order in Powder of Amorphous Anodic Yttrium Oxide L. A. Aleshina and S. V. Loginova Petrozavodsk State University, pr. Lenina 33, Petrozavodsk, 185640 Russia e-mail: [email protected] Received August 23, 2002 Abstract—The characteristics of the short-range order in a powder of amorphous yttrium oxide obtained by anodic oxidation are determined by the Finbak–Warren method. It is established that the first coordination num- ber equals seven. Amorphous oxide is built by irregular coordination polyhedra characteristic of the hexagonal and monoclinic modifications of yttrium oxide. © 2003 MAIK “Nauka/Interperiodica”. Yttrium oxide is widely used in planar optical is the convolution of the pair function Pij' (r) = devices for electroluminescent screens, in germanium- s max f (s)f (s)gÐ2(s)exp(Ð(α2 + σ 2 )s2)sin(sr )sin(sr)ds and silicon-based MIS varicaps and transistors, photo- ∫0 i j ij ij electric instruments, and nuclear technology. The oxide with the function of spreading of coordination spheres studied here is one of the most popular materials in in an amorphous material given in the form of a Gaus- micro- and optoelectronics and devices for displaying ()2 information. Thin films are also used as barriers, rr– ij Y2O3 sian G (r, r ) = Aexp–-------------------- . This representation efficient luminophor matrices, and dielectric interlay- ij ij σ 2 ers. ij allowed us to calculate the coordination numbers Nij by Amorphous Y2O3 oxide was studied in a limited the least squares method under the condition that number of publications [1]. The present study aimed to the radii of the coordination spheres rij are known. determine the short-range order characteristics of The method of these calculations was considered else- amorphous anodic Y2O3 oxide. We studied an amor- where [2]. phous yttrium oxide powder obtained by anodic oxida- tion. X-ray diffraction study of the samples was per- In the first approximation, the radii of the coordina- formed in reflection geometry on a DRON-4.0 diffrac- tion spheres were set based on the corresponding data for cubic yttrium oxide, the only phase which is stable tometer in automatic mode (Fe- and AgKα radiations). under normal conditions. The finite r and σ values A graphite monochromator was placed into a reflected ij ij beam. The maximum value of the diffraction vector s = were selected by the method of successive approxima- tions in such a way that the discrepancy between the 4πθsin ------------------ was 9.45 Å–1. observed curves and the curves calculated from the λ σ obtained set of Nij, rij, and ij curves did not exceed 5% [2–4]. All the necessary corrections were introduced into the experimental intensity-distribution curves [2–4]. It is well known that the cubic Y2O3 phase is related The recalculation to electron units was made by the to the Mn2O3 structure type (a = 10.6038 Å, sp. gr. Ia3) Warren method [5]. Figures 1a–1c show the intensity with the structure built by regular and distorted octahe- distribution curves I(s) in electron units; s-weighted dra [7] (Fig. 2a). The Y–O distance in regular octahedra interference functions H(s) multiplied by the attenua- equals 2.284 Å, the average distance in distorted octa- tion factor exp(Ðα2s2), where α = 0.1; and the distribu- hedra equals 2.282 Å, with the coordination number tion curves of pair functions D(r), respectively. The being equal to six. Nevertheless, the calculations details of the H(s) and D(r) calculation can be found showed that the Y–O distance in amorphous oxide is elsewhere [2, 4–6]. much larger, 2.39 Å, whereas the first coordination number equals seven. The Finbak–Warren representation [5, 6] of the D(r) curve as a sum of pair functions, Polymorphous transformations in RE metal oxides were studied elsewhere [8]. It was shown [9] that, with an increase in temperature, the structure of yttrium () Nij () Dobs r = ∑∑-------Pij r , oxide changes from cubic to hexagonal and, with an rij i j increase in pressure, from cubic to monoclinic. 1063-7745/03/4804-0531 $24.00 © 2003 MAIK “Nauka/Interperiodica” 532 ALESHINA, LOGINOVA H(s) I(s), el. units (a) 4000 (b) 2000 3000 2000 1500 1000 0 1000 Ð1000 500 Ð2000 123456789 123456789 s, ÅÐ1 s, ÅÐ1 D(r) (c) 15000 10000 5000 1234567 r, Å Fig. 1. Distribution of (a) scattered intensities, (b) the s-weighted interference function, and (c) pair functions for a powder of the yttrium oxide. The hexagonal phase is of the La2O3 structure type this distance is slightly overestimated (4.15 Å); in con- trast, the coordination number is underestimated in (sp. gr. P3m , a = 3.807 Å and c = 6.081 Å [9]). Figure 2b comparison with both phases and equals 6.5. shows the projection of six unit cells of this phase onto the ac plane. The Y–O distances in hexagonal yttrium The analysis of the next Y–O sphere (table) allows oxide are 2.36 and 2.6 Å for three oxygen atoms, 2.6 Å one to see the differences in the radii of coordination for three other oxygen atoms, while the seventh atom spheres and coordination numbers calculated for the lies at a distance of 2.43 Å from yttrium, so that the first cubic and hexagonal phases and the corresponding data coordination number equals seven and the average for the amorphous oxide. Thus, the cubic oxide has no shortest Y–O distance equals 2.47 Å, which exceeds the sphere characteristic of the amorphous oxide (4.88 Å). radius of the first coordination sphere in the amorphous The coordination number of this sphere in amorphous powder studied. oxide equals 2.90. At the same time, the cubic oxide has a sphere with r = 4.73 Å (c.n. = 7.54), which is absent The shortest Y–Y distance in cubic and hexagonal in both hexagonal and amorphous oxides. oxides is 3.52 and 3.56 Å, respectively. In the amor- phous oxide, this distance is considerably longer, The position of the Y–O sphere with r = 4.60 Å in 3.78 Å, despite the fact that the number of Y–Y pairs at the hexagonal oxide coincides with the position of the this distance corresponds to the respective data for the corresponding sphere in the amorphous oxide. How- cubic oxides (see table). The next Y–Y pairs are spaced ever, the coordination number of this sphere in the hex- at distances of 4.02 Å in the cubic oxide, but the contri- agonal modification is twice as high as the coordination bution to the electron density of this sphere also comes number of this sphere in the amorphous oxide. from the Y–O pairs, so that the average weighted radius The next Y–O sphere (5.09 Å) in the hexagonal equals 4.12 Å and the coordination number calculated oxide is displaced toward larger r values with respect to from the area under the sum of pair functions PYÐY and the corresponding value for the powder oxide. The coordination number of this sphere (4.84) is overesti- PYÐO by the methods suggested in [2] equals 7.5. In the hexagonal oxide, the contribution to the corresponding mated in comparison with the data for the amorphous sphere also comes from the Y–O pairs; therefore the oxide (6.10). average weighted radius equals 3.85 Å and the coordi- The Y–Y sphere in the cubic and hexagonal oxides nation number equals 9.34. In the amorphous oxide, (5.35 and 5.36 Å, respectively) is displaced toward CRYSTALLOGRAPHY REPORTS Vol. 48 No. 4 2003 SHORT RANGE ORDER IN POWDER 533 c b (a) (b) Y atom, y = 0.333 Y atom, z = 0.25 Y atom, y = 0.667 O atom, z = 0.3827 O atom, y = 0.667 O atom, z = 0.1516 O atom, y = 0.333 O atom, z = 0.3911 O atom, y = 0.0 O atom, z = 0.1173 O atom, z = 0.3484 O atom, z = 0.1089 a a c (c) Y atom, y = 0.0 Y atom, y = 0.5 O atom, y = 0.5, y = Ð0.5 O atom, y = 0.0, y = 1.0 a (d) Fig. 2. Atomic arrangements in various modifications of yttrium oxide projected onto the ac plane: (a) cubic, (b) hexagonal, (c) monoclinic modification, and (d) coordination polyhedra for three yttrium atoms in the model of the monoclinic Y2O3 phase. smaller r values in comparison with the corresponding spheres and coordination numbers for monoclinic value for the amorphous oxide. The coordination num- yttrium oxide. The monoclinic phase is of the Sm2O3 bers of this sphere are practically equal for both crystal- structure type [9–11] (Fig. 2c). The atomic coordinates line and amorphous modifications. of the monoclinic Y2O3 are unknown, and, therefore, The study of deposited films [1] showed that the the unit cell of this phase was constructed based on the specific feature of the formation of the short-range data for Sm2O3 and the transition to the lattice of mon- order in their structures is the appearance of the mono- oclinic Y2O3. The atoms were located in the basic group clinic phase and an increase in its relative content in proceeding from crystallochemical considerations. Fig- comparison with the content of the cubic phase with an ure 2d shows the coordination polyhedra of three increase in the oxygen content in the atmosphere during yttrium atoms.
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