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19PHYSICS AND MATHEMATICS
STUDY OF THE STRUCTURE OF THE BUKHARA METEORITE
Yuldashev B.,
ChiefResearcher of the Institute of Nuclear Physics of the Academy of Sciences of the Republic of Uzbekistan, Academician Ehgamberdiev Sh.,
Director of the Astronomical Institute of the Academy of Sciences of the Republic of Uzbekistan,
Academician Tashmetov M.,
Deputy Director of the Institute of Nuclear Physics of the Academy of Sciences of the Republic of Uzbekistan, Professor
Ismatov N.,
Senior researcher at the Institute of Nuclear Physics of the Academy of Sciences of the Republic of Uzbekistan
Yuldashova I.
Junior researcher at the Institute of Nuclear Physics of the Academy of Sciences of the Republic of Uzbekistan
DOI: 10.5281/zenodo.6882545
Abstract
The structure and structural characteristics of the minerals present in the meteorite, which fell into Bukhara (Uzbekistan) in 2001, were determined by X-ray diffraction technique. Within the resolution of the Empyrean diffractometer, the following phases were found to exist in the meteorite: tetrataenite, jadeite, calcite, troilite, au-gite, fayalite, pygeonite, and fassaite. It was found that Fassaite is described in a monoclinic unit cell (space group C2/c), in which Ca, Mg, Fe, Al, Ti, and Si atoms are displaced from ideal positions. Lattice parameters of were determined jadeite Na(Al0.74Fe0.26)Si2O6 included in the pyroxene group with a monoclinic structure (space group C2/c) of the sample of the Bukhara meteorite are lower than in other literature. It can be assumed that this is due to the high pressure formed when the meteorite enters the Earth's atmosphere. The sizes of the fayalite and jadeite crystallites in the meteorite sample are 18.22 and 28.89 nm, respectively.
Keywords: meteorite, X-ray diffraction, crystal structure, unit cell, structural phase.
Introduction
Currently, the world has collected a collection of about 30000 meteorites [1], which contain information about the elements and minerals that exist in space objects. Minerals of meteorites mainly contain iron, silicon, magnesium, aluminum, oxygen, sodium, calcium, potassium, and in small amounts from less abundant elements such as sulfur, chromium, phosphorus, carbon and titanium [2]. Studies of meteorites have established the presence of about 295 minerals in them [3]. Based on the study of the meteorite composition of the minerals present and their crystal structure, it is possible to predict where the meteorite came from. The availability of data on meteorites also makes it possible to draw up a map of the elements, minerals available in space objects, which makes it possible to expand the understanding not only of meteorites, but also, in rough approximations, of the existing or existing conditions in a particular space object, from where it broke away and flew to Earth. One of these is the meteorite discovered in 1984 in Antarctica [4, 5] and which, according to experts, is a breakaway rock from the planet Mars. Studies of meteorite samples [4, 5] have established the presence of orthopyroxene, augite, maskelinite, chro-mite, TiO2, Fe2O3 and also suggested the existence of biological objects on Mars in the distant past. The study of the meteorite is mainly devoted to the determination of the elemental composition and minerals.
Another important aspect of the study of meteorites is that when entering the earth's atmosphere at high speed due to pressure and high temperature, various crystallographic structures are formed, phase transitions occur, the production and study of which in research laboratories requires the creation of certain conditions. For example, the speed of movement of the Tunguska meteorite when it collided with the Earth, according to [6], was 20 km per second, and the pressure and heating temperature are very high (above 20000C), which is difficult to create in laboratory conditions. Considering the interconnectedness of the structure and properties of materials, it is of interest to study the structure of meteorite minerals.
Studies of the Suizhou meteorite, discovered in Suizhou (China, 1986), found that the meteorite contains mainly &2O3 (56-57 wt%), FeO (29 wt%), as well as a small amount of A^O3, MgO, TiO2, MnO and V2O3 [7]. On the basis of measurements at the synchrotron, the existence of a FeCr2O4 phase with a sort with an orthorhombic structure [7], as well as a polymorphic phase transformation of this phase at a pressure of 2023 GPa and temperatures of 1800-20000C [7] was established. In a meteorite [8] (Bruderheim, Canada), the presence of minerals consisting of the following phases was established: forsterite, trolite (troilite-2H), as well as enstatite, in which the atoms are in an ordered state. However, in [8], the parameters of unit cells, atomic coordinates, site populations are not given, and phases
(kamacite, orthopyroxene, clinopyroxene, plagioclase) found in 10 other meteorites are not discussed. The crystal structure of some phases, grain sizes, stress were investigated in [9] on five meteorites and in one of the Martian meteorites the presence of forsterite was established - (Mgi.2i5Feo.785)SiÜ4 with orthorhombic structure (space group Pbnm), pygonite (pigeonite) -(Cao.i8Mgi.2iFeo.58)(SiÜ3)2 with a monoclinic structure (space group P21/c). In the samples of the Tenham meteorite (Australia), the existence at high pressures of a phase transition from orthoenstatite (space group Pbca) to clinoenstatite (space group P21/c) through the formation of the intermediate monoclinic phase clinoen-statite (space group C2/c) [10]. X-ray diffraction studies of carbonaceous-chondrite meteorites established [11] the existence of olivine, enstative, Fe-cronstedtite, Mg-serpentine, calcite, magnetite, Fe-sulphide, and the content of each mineral was determined. The existence of complex minerals in the meteorite (NaNa2Mg3Fe2+o.5Ti1.5(Si8Ü22)Ü2; Na2Mg5TiSi6Ü18Ü2; Na(Mg,Fe)o.5Tio.5Si2Ü6) was discovered in [12], in which, according to the authors, a more detailed structural study should be carried out. In [13], the Chelyabinsk meteorite was studied using the neutron diffraction method and the existence of a body-centered cubic phase (space group Im-3m), orthorhombic phases (space group Pbnm; Pbca), a hexagonal phase (space group P-62c) and triclinic phase (space group P-1). It should be noted that the existence of FeS and the body-centered phase -Fe was also established in [13]. And also [14] established the mechanism of formation of the crystalline phase (FeNi) in carbonaceous chondrites CV3 (Bali meteorite). In [15], the presence of plagioclase, nepheline, jadeite, kamasite, troilitetaenite, pygeonite, augite, and fassaite in a meteorite that fell into Bukhara (Uzbekistan) on July 9, 2oo1 was reported.
It should be noted that the study of the structure of each meteorite is interesting in that they are original not only in composition, content of elements, crystal structure, but also in that they provide unique information about the effect of temperature and pressure on structures, phase formation and phase transitions. Another feature of minerals is that a change in the content of elements, partial and complete replacement of some of them with another element can lead to a change in the structure. For example, the compound KNa3Mn7(PÜ4)6 has a monoclinic structure (space group C2/c), NaMg4(PÜ4)3 corresponds to the orthorhombic phase (space group Pnma), and NaCo4(PÜ4)3 has a monoclinic structure (space group P21/n) [16].
In [17], using micro-Raman spectroscopy, the sizes of crystallites of the Allende and Bali meteorites, which belong to the group of carbonaceous chondrites CV3, were studied. It was found that the average value of the crystallite size for the Allende meteorite is 13.64 nm, and for the Bali meteorite 14.85 nm [17].
It is assumed that chondrites were formed from the substance of a protoplanetary cloud that surrounded the Sun [18]. They were episodically subjected to heating and, at the same time, some structural and mineralogi-
cal changes occurred in them [18]. The Bukhara meteorite, as well as [19, 20, 21, 22, 23], refers to carbonaceous chondrites (group CV3). A content of Noble gases and nitrogen in CV3 chondrite Bukhara was published in [24]. In [23], the subgroup to which the Bukhara meteorite belongs was established, and the magnetic susceptibility, Raman and infrared spectroscopy of the meteorite were also studied. However, the structures, unit cell parameters, crystallite size and atomic coordinates of the observed phases [15] were not reported. Structural studies have not been carried out in [23, 24], although such data can provide information to make an assumption about the origin of the meteorite, the conditions for the coexistence of various phases, the mechanisms of formation and the possibility of growth of nanocrystallites, etc.
Thus, the purpose of this study is to study the crystal structure of minerals, and their parameters contained in the meteorite, which was discovered in Bukhara in 2001.
Experimental details
X-ray structural studies were carried out on a Pan-alytical Empyrean diffractometer in the range 29b=20.04-70.01°, with a step of 0.0070, and a recording rate of 0.017 deg/min. at a copper tube current of 45 mA and a voltage of 40 kV. In the experiment, a powder sample of the Bukhara meteorite was used, the X-ray diffraction pattern was taken with the rotation of the sample in order to exclude the effect of texture on the diffraction pattern.
The structure of the measured X-ray diffraction pattern was identified by processing the results obtained by the Rietveld method [25] using the FullProf program.
Calculations were made to determine the size of crystallites by Scherrer formula [26]:
D K
Ps cos 0
where, K is a correction factor for taking into account the grain shape (K~ 0.9), X is the radiation wavelength (for example, 0.15406 nm), 0 is the Bragg angle for the diffraction peak, Ps is the observed width at half height of the peak (in radians).
Experimental results
To decipher the crystallographic structures of the compounds (phases) present in the meteorite, calculations were performed under the assumption of the formation, as in [15, 27-48] of the following minerals: MgCo(SiO4), Fe2SiÛ4, (MgFe)2SiÛ4, SiMgOs, SiO2, SiC, (AlSis) (Nao.667Ko.333)O8, FeS, Fe2SiO4, FeN, NisFe, FeO, FefeO4, FesO4, FesNi, FefeS4, (FeNi)sC, (FeNi)2P, FeSi, FesC, MgO, FeO, MnO, CaO, A^Os, &2O3, Al2O3, K2O, Na2O, CrN, CaNa8, CaCOs, Ca4Na4, CaAl4O7, Ca(Si2Al2)O8,
Ca(MgFeAl)(SiAl)2O6, ZnC^, K4CaSi3O8, NaS6, (MgFeCa)CO3.
The calculated data showed that relatively good agreement (x2 = 2.35) between the experimental data and the proposed structures is achieved in the presence of eight phases in meteorite (Fig. 1).
1100
25 35 45 55 65
20 O
Fig. 1. X-ray diffraction pattern of the Bukhara meteorite, consisting of I-; II-; HI-; IV-; V-; VI-; VII-; VIII-phase. 1 - ■■■■ experimental, — calculated; 2 - Bragg peaks; 3 - the difference between experimental and calculated data.
X-ray data calculations have shown that the mete- in which there are iron atoms in two, silicon atoms in orite contains fayalite (Fe2SiO4) and has an orthorhom- one, and oxygen in three crystallographic positions. bic structure (space group Pbnm) (Fig. 2) with lattice
parameters o=4.7923 A; 6=10.3696 Aandc=6.0415 A,
Fig. 2. Crystal structure (Fe2SiO4).
The results of calculations carried out under the assumption of the existence of calcite CaCO3 with a tri-clinic cell (space group P1) showed good agreement between the model and experimental data (x2 = 1.60).
Calculations based on the data from [15] showed that, as in [44], augite, belonging to the pyroxene group,
is also present in the meteorite sample. Augite corresponds to the composition (CaMg0.74Fe0.25) Si2Ö6, which has a monoclinic structure (Fig. 3) (space group C2/c) with unit cell parameters: a=9.7593 Â; è=8.8567 Â; c=5.2984 Â and ,0=106.24°.
(CaMgo.74Feo.25)Si206
Fig. 3. Crystal structure of (CaMgo.7Feo.25) Si2O6.
In this structure, some of the iron atoms are re- oxygen atoms in three positions. The atomic coordi-placed by magnesium atoms, silicon atoms in one, and nates of augite (CaMgo.74Feo.25)Si2O6 are given in Table
1.
Table 1.
Coordinates of augite atoms (CaMgo.74Feo.25)Si2O6 in the Bukhara meteorites monoclinic structure (space group C2/c)._
Atoms Atomic coordinates
X y z
Ca2 0.0000 0.4977 0.2500
Mg1 0.0000 0.9127 0.2500
Fe1 0.0000 0.9012 0.2500
Si 0.4934 0.0652 0.2873
O1 -0.0126 0.2227 -0.2260
O2 0.1822 0.3078 0.3722
O3 0.3821 0.0814 -0.5819
In the studied sample of the Bukhara meteorite is fassaite with a complex composition
Na0.09Ca0.6i6Mg0.902Fe0.21Al0.342Ti0.02Si1.82O6, which is described in a monoclinic unit cell (space group C2/c).
In this unit cell (Fig. 4) with a=9.6397 Â, 6=8.8271 Â and c=5.2639 Â, atoms (Ca; Mg; Fe; Al; Ti; Si) are displaced from ideal positions.
Fig. 4. Crystal structure of fassaite Na0.09Ca0.616Mg0.902Fe0.21Al0.s42Ti0.02Si1.82O6.
Also in Bukhara meteorite were determined following minerals: tetrataenite (FeNi) with a tetragonal structure, pygonite Fe1.0œMg0.871Ca0.m(Si1.98Al0.02)O6
with a monoclinic structure, troilite (FeS) with a hexagonal structure and jadeite Na(Alo.74Feo.26)Si2O6 with a monoclinic structure.
For determine the size of crystallites were chosen the reflections at 22.6134° and 31.7162° correspond to
fayalite and jadeitec, and there is almost no contribution from reflections of other phases (Figure 1) to their intensity. The performed calculations showed that the sizes of fayalite and jadeite crystallites in the meteorite sample are 18.22 and 28.89 nm, respectively.
Discussion
The X-ray diffraction pattern shows that the peak full width at half maximum (FWHM) is relatively wide. For example, the FWHM of the reflection at 20b = 31.03340 determined by fitting the shape of the reflection using the Lorentz function is 0.24070, which indicates that the sample has undergone rapid quenching, retaining its high-temperature state. Comparison of the X-ray diffraction pattern with the data [11] showed the presence of some differences, consisting not only in the scattering angles, but also in the intensity of individual reflections. For example, the most intense reflex of the present experiment corresponds to the scattering angle 20b~31.69560, and in [11] 20b~31°. And the reflex with 20b~51.8136° found in this work is relatively higher in intensity than the similar reflection in [11]. The reflection with 20b~6O0 present in [11] is absent in this work, but just as in [11] there are reflections with different intensities in the range 20b~56° - 580.
Metal atoms of (Fe, Si) at fayalite are displaced from ideal positions, which, in contrast to [49], are not associated with the replacement of some iron atoms with magnesium and manganese atoms, but most likely with rapid quenching from high temperatures.
It is determined that all CaCO3 atoms in the unit cell are in ideal positions, which may be due to the fact that calcite was formed already on the Earth during cooling at relatively low temperatures. Although, according to the authors of [32], the discovered calcite CaCO3 was present on the meteorite before reaching the Earth's surface.
It should be noted that the calculations of X-ray diffraction patterns in the presence of a forsterite (Mg2SiO4) sample as well as in [36] of the orthorhom-bic (space group Pbnm) phase, as well as in [37] of the triclinic (space group P1) phase did not give good agreement with the proposed a model with experimental data, which is expressed in the inconsistency of the angular positions of the reflections.
Taking into account the data [45] on the existence of the mineral (MgFeCa)CO3 in the Martian meteorite, the presence of monoclinic [46] (space group P21/c), orthorhombic [47] (space group Pmcn), triclinic ( space group P1) [48] of the structures, X-ray diffraction patterns were calculated. Calculations showed that the quality of the X-ray diffraction pattern fitting in each of the unit cells according to the data [46-48] is a low, in which the calculated intensities of the reflections are higher than the experimental ones.
Jadeite Na (Al0.74Fe0.26)Si2O6 included in the pyroxene group with a monoclinic structure (space group C2/c), as in [41], is also present in the sample of the Bukhara meteorite, which corresponds to the composition Na(Al0.74Fe0.26)Si2O6, and the unit cell has the following parameters: a=9.3985 A; b=8.4719 A and c=5.2026 A. Silicon atoms are located in tetrahedral with coordinates x=0.38935, y=0.13071 and z=0.32266. The lattice parameters are lower than in
[50] (a=9.42330 A; b=8.56511 A; c=5.22346 A at 270 K), which is not associated with the replacement of some aluminum atoms with iron atoms, since the atomic radius of iron is greater than that of aluminum. However, it can be assumed that this is due to the high pressure formed when the meteorite enters the Earth's atmosphere.
In the meteorite sample, as in [40], pygonite Fe1.008Mg0.871Ca0.121(Si1.98Al0.02)O6 with a monoclinic structure (space group P21/c) and cell parameters a=9.8059 A; b=8.8484 A; c=5.2261 A was found, which differ from the data [51], which is due to the difference in the content of iron, magnesium, and calcium in the samples. In this structure (space group P21/c), magnesium atoms replace part of iron atoms and are located in two positions, and aluminum atoms replace part of silicon atoms and also occupy two positions in the crystal structure. The presence of the second phase in the pygonite phase (space group C2/c), established in [52] with the application of high pressure (3.6 GPa), was not revealed in the Bukhara sample.
Tetrataenite (FeNi) [42] found in a sample of the Bukhara meteorite with a tetragonal structure (space group P4/mmm) as well as [53] has a=2.5330 A; b=2.5330 A; c=3.5820 A, in which the iron atoms with (0,0,0) and nickel with (0.5,0.5,0.5) coordinates are in ideal positions. The present data support the results.
Troilite (FeS) [43] with a hexagonal structure (space group P-62c) is present in the sample of the Bukhara meteorite; the work (a=5.9891 A; b=5.9891 A; c=11.7339 A) and in [54] (a=b=5.9650 A; c = 11.7570 A).
In the Bukhara meteorite, as in [38, 39], there is fassaite with monoclinic unit cell and displacement of atoms from ideal positions is most likely due to the rapid quenching of the sample from high temperature.
The sizes of fayalite and jadeite crystallites (18.22 and 28.89 nm, respectively) in the Bukhara meteorite are closer to the size of Allende and Bali fayalite crystallites [17].
Thus, within the limits of the sensitivity of the method of X-ray structural analysis, the possibility of resolving the X-ray diffraction device, the presence of eight phases was found in the Bukhara meteorite.
Conclusion
X-ray diffraction analysis of the Bukhara meteorite revealed the presence of calcite (CaCO3), augite ((CaMg0.74Fe0.25)Si2O6), fassaite
(Na0.09Ca0.616Mg0.902Fe0.21Al0.342Ti0.02Si1.82O6), jadeite (Na(Al0.74Fe0.26)Si2O6), pygeonite
(Fe1.008Mg0.871Ca0.121(Si1.98Al0.02)O6), tetrataenite (FeNi), troilite (FeS) and fayalite (Fe2SiO4).
In calcite CaCO3 with a triclinic structure (space group P1) and tetrataenite (FeNi) with a tetragonal structure (space group P4/mmm), atoms are in ideal crystallographic positions.
It was found that the pygonite Fe1.008Mg0.871Ca0.121(Si1.98Al0.02)O6 has a monoclinic structure (space group P21/c) with unit cell parameters a=9.8059 A, b=8.8484 A and c=5.2261 A.
Troilite (FeS) with a hexagonal structure (space group P-62c) is present in the sample of the Bukhara
meteorite, in which the positions of iron and sulfur are completely filled.
It was found that jadeite Na(Al0.74Fe0.26)Si2O6 belongs to the monoclinic structure (space group C2/c) with the unit cell parameters a=9.3985 A; 6=8.4719 A and c=5.2026 A.
Fassaite
Na0.09Ca0.616Mg0.902Fe0.21Al0.342Ti0.02Si1.82O6 is described in a monoclinic cell (space group C2/c), in which Ca, Mg, Fe, Al, Ti, and Si atoms are displaced from ideal positions.
It was found that the structure of augite (CaMg0.74Fe0.25)Si2O6) belongs to the monoclinic system (space group C2/c) with a=9.7593 A; b=8.8567 A; c=5.2984 A and ^=106.24°.
It was shown that fayalite (Fe2SiO4) has a ortho-rhombic structure with a=4.7923 A; b=10.3696 A and c=6.0415 A, in which there is no isomorphic substitution of iron atoms for magnesium atoms.
It is established that the size of fayalite and jadeite crystallites in the Bukhara meteorite sample is 18.22 and 28.89 nm, respectively.
Acknowledgments
The authors are grateful to B.A. Abdurakhimov and F.K. Khallokov for his help in carrying out experiments on the Empyrean X-ray diffraction apparatus and calculations.
The study was carried out as part of the research program of the Institute of Nuclear Physics of the Academy of Sciences of the Republic of Uzbekistan for 2020-2024, on the topic "Radiation-stimulated processes during nuclear transmutation of doped mono-crystalline silicon" in the laboratory of radiation physics and technology of solid-state electronics.
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