Magnetic phase transitions in the system La₁₋xBixMnO₃₊λ

The crystal structure and magnetic properties of the La₁₋xBixMnO₃₊λ system (0⩽x⩽1;λ⩽0.08) are studied as functions of the oxygen and bismuth contents. In oxidized samples La₁₋xBixMnO₃₊λ a phase transition from a ferromagnetic state (rhombohedric phase) to a state of the spin glass type (quasitetrago...

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Hauptverfasser: Troyanchuk, I.O., Mantytskaja, O.S., Szymczak, H., Shvedun, M.Yu.
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Veröffentlicht: Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України 2002
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spelling nasplib_isofts_kiev_ua-123456789-1302362025-02-09T14:07:37Z Magnetic phase transitions in the system La₁₋xBixMnO₃₊λ Troyanchuk, I.O. Mantytskaja, O.S. Szymczak, H. Shvedun, M.Yu. Дефекты в кристаллах The crystal structure and magnetic properties of the La₁₋xBixMnO₃₊λ system (0⩽x⩽1;λ⩽0.08) are studied as functions of the oxygen and bismuth contents. In oxidized samples La₁₋xBixMnO₃₊λ a phase transition from a ferromagnetic state (rhombohedric phase) to a state of the spin glass type (quasitetragonal phase) is observed with increase of the bismuth concentration. The reduced samples La₁₋xBixMnO₃ are weak ferromagnets down to x⩽0.6 and then transform into a ferromagnetic state. It is supposed that the Bi³⁺ ions stabilize the dx2−y2 orbitals in the nearest Mn³⁺ ions whereas the dz2 orbitals of the La³⁺ ions are stabilized. The orbitally disordered phases and dx2−y2-orbitally ordered phases are ferromagnetic, the dz2-orbitally ordered phases show antiferromagnetic ordering, and the state of the orbital glass type corresponds to a state of the spin glass type. The crystal structure and magnetic properties of the La₁₋xBixMnO₃₊λ system (0⩽x⩽1;λ⩽0.08) are studied as functions of the oxygen and bismuth contents. In oxidized samples La₁₋xBixMnO₃₊λ a phase transition from a ferromagnetic state (rhombohedric phase) to a state of the spin glass type (quasitetragonal phase) is observed with increase of the bismuth concentration. The reduced samples La₁₋xBixMnO₃ are weak ferromagnets down to x⩽0.6 and then transform into a ferromagnetic state. It is supposed that the Bi³⁺ ions stabilize the dx2−y2 orbitals in the nearest Mn³⁺ ions whereas the dz2 orbitals of the La³⁺ ions are stabilized. The orbitally disordered phases and dx2−y2-orbitally ordered phases are ferromagnetic, the dz2-orbitally ordered phases show antiferromagnetic ordering, and the state of the orbital glass type corresponds to a state of the spin glass type. This work was supported in part by the Belarus Fund of Basic Research (Project F00-223). 2002 Article Magnetic phase transitions in the system La₁₋xBixMnO₃₊λ / I.O. Troyanchuk, O.S. Mantytskaja, H.Szymczak, M.Yu. Shvedun // Физика низких температур. — 2002. — Т. 28, № 7. — С. 790-795. — Бібліогр.: 28 назв. — англ. 0132-6414 PACS: 72.15.Gd, 75.30.Kz, 75.70.Pa https://nasplib.isofts.kiev.ua/handle/123456789/130236 en Физика низких температур application/pdf Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України
institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
collection DSpace DC
language English
topic Дефекты в кристаллах
Дефекты в кристаллах
spellingShingle Дефекты в кристаллах
Дефекты в кристаллах
Troyanchuk, I.O.
Mantytskaja, O.S.
Szymczak, H.
Shvedun, M.Yu.
Magnetic phase transitions in the system La₁₋xBixMnO₃₊λ
Физика низких температур
description The crystal structure and magnetic properties of the La₁₋xBixMnO₃₊λ system (0⩽x⩽1;λ⩽0.08) are studied as functions of the oxygen and bismuth contents. In oxidized samples La₁₋xBixMnO₃₊λ a phase transition from a ferromagnetic state (rhombohedric phase) to a state of the spin glass type (quasitetragonal phase) is observed with increase of the bismuth concentration. The reduced samples La₁₋xBixMnO₃ are weak ferromagnets down to x⩽0.6 and then transform into a ferromagnetic state. It is supposed that the Bi³⁺ ions stabilize the dx2−y2 orbitals in the nearest Mn³⁺ ions whereas the dz2 orbitals of the La³⁺ ions are stabilized. The orbitally disordered phases and dx2−y2-orbitally ordered phases are ferromagnetic, the dz2-orbitally ordered phases show antiferromagnetic ordering, and the state of the orbital glass type corresponds to a state of the spin glass type.
format Article
author Troyanchuk, I.O.
Mantytskaja, O.S.
Szymczak, H.
Shvedun, M.Yu.
author_facet Troyanchuk, I.O.
Mantytskaja, O.S.
Szymczak, H.
Shvedun, M.Yu.
author_sort Troyanchuk, I.O.
title Magnetic phase transitions in the system La₁₋xBixMnO₃₊λ
title_short Magnetic phase transitions in the system La₁₋xBixMnO₃₊λ
title_full Magnetic phase transitions in the system La₁₋xBixMnO₃₊λ
title_fullStr Magnetic phase transitions in the system La₁₋xBixMnO₃₊λ
title_full_unstemmed Magnetic phase transitions in the system La₁₋xBixMnO₃₊λ
title_sort magnetic phase transitions in the system la₁₋xbixmno₃₊λ
publisher Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України
publishDate 2002
topic_facet Дефекты в кристаллах
url https://nasplib.isofts.kiev.ua/handle/123456789/130236
citation_txt Magnetic phase transitions in the system La₁₋xBixMnO₃₊λ / I.O. Troyanchuk, O.S. Mantytskaja, H.Szymczak, M.Yu. Shvedun // Физика низких температур. — 2002. — Т. 28, № 7. — С. 790-795. — Бібліогр.: 28 назв. — англ.
series Физика низких температур
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AT szymczakh magneticphasetransitionsinthesystemla1xbixmno3l
AT shvedunmyu magneticphasetransitionsinthesystemla1xbixmno3l
first_indexed 2025-11-26T15:23:23Z
last_indexed 2025-11-26T15:23:23Z
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fulltext Fizika Nizkikh Temperatur, 2002, v. 28, No. 7, p. 790–795 Magnetic phase transitions in the system La1–xBixMnO3+� I. O. Troyanchuk and O. S. Mantytskaja Institute of Solid State and Semiconductor Physics of National Academy of Sciences of Belarus 17 P. Brovki Str., Minsk 220072, Belarus E-mail: troyan@ifttp.bas-net.by H. Szymczak Institute of Physics of Polish Academy of Sciences 32/46 Al. Lotnikow Str., Warsaw PL-02-668, Poland M. Yu. Shvedun B. Verkin Institute for Low Temperature Physics and Engineering of the National Academy of Science of Ukraine, 47 Lenin Ave., Kharkov 61103, Ukraine Received January 4, 2002 The crystal structure and magnetic properties of the La1-xBixMnO3+� system ( ;0 1� �x � � 008. ) are studied as functions of the oxygen and bismuth contents. In oxidized samples La1–xBixMnO3+� a phase transition from a ferromagnetic state (rhombohedric phase) to a state of the spin glass type (quasitetragonal phase) is observed with increase of the bismuth concentration. The reduced samples La1–xBixMnO3 are weak ferromagnets down to x � 06. and then transform into a ferromagnetic state. It is supposed that the Bi3 + ions stabilize the dx y2 2� orbitals in the nearest Mn3+ ions whereas the dz2 orbitals of the La3+ ions are stabi- lized. The orbitally disordered phases and dx y2 2� — orbitally ordered phases are ferromag- netic, the dz2 — orbitally ordered phases show antiferromagnetic ordering, and the state of the orbital glass type corresponds to a state of the spin glass type. PACS: 72.15.Gd, 75.30.Kz, 75.70.Pa Introduction Recently considerable interest has been attracted to strongly correlated systems with perovskite-like structure. The variety of triple perovskites such as RMO3 (R is a rare-earth metal, M is a transition metal) is quite great, but with variation of the rare-earth element (R = La, Pr, Nd etc.) and the addition of the practically unlimited set of solu- tions R1–xAxMnO3, the number of combinations becomes extremely large. Manganites R1–xAxMnO3 have interesting and unusual properties. These compounds contain ions with orbital degeneracy or Jahn–Teller (JT) ions (in our case Mn3+) [1]. Thus their properties differ appreciably from those of the corresponding sub- stances with the «ordinary» ions: the crystal structure turn out to be distorted, structural phase transitions and transitions in a magnetic subsystem [2–6] are frequently observed in them, and in many cases they have anomalously strong magnetic aniso- tropy and magnetostriction [7,8]. Such phenomena are connected with an interaction of the JT ions and are called the cooperative Jahn–Teller effect (CJTE). Distortions of the crystal lattice are caused by the fact that ion Mn3+ is degenerate with respect to the d orbitals: the crystal field splits the atomic d level into two- and threefold degenerate sublevels eg and t2g (the eg state is characterized by the real wave functions dz2 and dx y2 2� ). The first of them lies above the second one, and conse- quently the four d electrons of the Mn3+ ion occupy © I. O. Troyanchuk, O. S. Mantytskaja, H. Szymczak, and M. Yu. Shvedun, 2002 the level t2g completely and the level eg only in part. This also makes CJTE possible, which reduces the energy of such a degenerate system by lowering its symmetry, which lifts the degeneracy of the electronic levels. Despite the numerous works devoted to research on manganites, many problems remain subject to discussion. The unusual magnetic behavior of bis- muth-containing manganites is one such problem. While the lanthanum-based manganites (Ln–La, Y, rare-earth ion) are antiferromagnetic [9], bismuth manganite is a ferromagnetic insulator [10,11]. Mo- reover, while substitution of the lanthanoid by an alkaline-earth metal leads to a transition from the antiferromagnetic to a ferromagnetic metallic state [12], a similar substitution for BiMnO3-based man- ganites destroys the ferromagnetic order [13–15]. The aim of the present work is to study phase transitions in a system of manganites where La3+ ions are replaced by Bi3+ ions. Formally upon such a substitution the valence of the manganese ions should not change. Experiment Samples of the La1-xBixMnO 3+� system were obtained by three different methods: in air, under a high pressure, and in vacuum. The initial reagents were oxides of La2O3, Bi2O3 and Mn2O3, mixed in the desired proportion. The manganite of lantha- num was obtained at Ò = 1500 °C in air. Synthesis of Bi-containing samples was carried out in the temperature range of 900–1150 °C with a subse- quent slow cooling (100 °C/h). The temperature of synthesis decreased with increasing bismuth con- tent from 1150 °C (x � 0.2) to 900 °Ñ (x � 0.7). Ac- cording to x-ray phase analysis, in a sample with x � 0.7 there were traces of extraneous phases; therefore in these states the saturated concentration of bismuth is limited to a value of 65%. A chemical analysis has shown that all compounds obtai- ned in air have an excess of oxygen in comparison with the stoichiometric ratio. Substitution of the La3+ ions by Bi3+ has only a weak influence on the oxygen content. The chemical formula is La1-xBixMnO3.07±0,01. The samples prepared by the method described were reduced in quartz vacuum tubes at 900 °Ñ in the presence of tantalum metal for absorption of allocated oxygen. Control of the oxygen maintenance was carried out by mass weighing of the sample before and after the reduc- tion process. The chemical formula was «squared up» on loss of the mass. Compounds with x � 0.7 were obtained using a high-pressure technique (pressure 4 GPa, temperature 900 °Ñ, duration of synthesis 20 min). These samples were characterized by the chemical composition La1-xBixMnO3±0,01. X-ray structure studies were carried out on a DRON-3 diffractometer in Cr K � radiation. Sing- le-phase structures were selected for measurement of the magnetic and electric properties. Magnetic measurements were carried out on a commercial vi- brating Foner magnetometer. The electroconduc- tivity was measured by a standard four-probe techni- que. Indium contacts were used. They were applied using ultrasound. Results and discussion According to the x-ray data, the samples of the La1–xBixMnO3.07 series obtained in air were cha- racterized by rhombohedral distortions of the unit cell up to a concentration x � 0.4. In samples with x � 0.5 the type of distortions changed to tetra- gonal. The compounds reduced in vacuum and ob- tained under a high pressure had a monoclinic or orthorhombic deformed unit cell. Upon substitution of lanthanum by bismuth, the volume of the unit cell varied only slightly, appa- rently because of the similarity of the ionic radii of Fizika Nizkikh Temperatur, 2002, v. 28, No. 7 791 Magnetic phase transitions in the system La1–x Bi x MnO3+� Table 1 Unit cell parameters of La1–xBixMnO3,07 compounds obtained in air Composition Symmetry a, Å c, Å �, deg V, Å3 LaMnO 3.07 R 7.8105 — 90.46 59.55 La 0.8 Bi 0.2 MnO 3.07 R 7.8165 — 90.45 59.69 La 0.7 Bi 0.3 MnO 3.07 R 7.8191 — 90.34 59.75 La 0.6 Bi 0.4 MnO 3.07 R 7.8198 — 90.27 59.7 La 0.5 Bi 0.5 MnO 3.07 T 3.9098 3.9352 — 60.156 La 0.4 Bi 0.6 MnO 3.07 T 3.9048 3.9409 — 60.09 La3+ and Bi3+. The unit cell parameters of some solid solutions are given in Tables 1 and 2. Accor- ding to structural studies [16], the excess over stoi- chiometric oxygen in the system LaMnO3+� is a consequence of the formation of an equivalent num- ber of vacancies of La3+ and Mn3+ ions. Apparently this mechanism of nonstoichiometry is pertinent to system La1-xBixMnO 3+� also, as the oxygen ions cannot occupy interstitial positions in the close- packed perovskite structure. Field curves of the magnetization M(H) at liquid helium temperature for several samples prepared in air are shown in Fig. 1. LaMnO3,07 is ferromag- netic, as the specific magnetization corresponds to a parallel orientation of the magnetic moments of the manganese ions. With increase of the bismuth con- tent up to x � 0.65, a gradual decrease of the spon- taneous magnetization was observed. In compounds with x � 0.6 and x � 0.65 the magnetization remains unsaturated in fields up to 16 kOe, as is typical for 792 Fizika Nizkikh Temperatur, 2002, v. 28, No. 7 I. O. Troyanchuk, O. S. Mantytskaja, H. Szymczak, and M. Yu. Shvedun Fig. 2. Temperature dependence of the magnetization in the La1-xBixMnO3.07 system (ZFC curve — filled sym- bols, FC — unfilled symbols). Fig. 3. Magnetic field dependence of the magnetization in the La0.5Bi0.5MnO3+� system. Fig. 4. Temperature dependence of the magnetization in the La0.5Bi0.5MnO3+� system (ZFC curve — filled sym- bols, FC — unfilled symbols). Fig. 1. Magnetic field dependence of the magnetization in the La1-xBixMnO3.07 system. Table 2 Unit cell parameters of La1–xBixMnO3+� compounds obtained in vacuum Composition Symmetry a, Å b, Å c, Å V, Å3 La 0.5 Bi 0.5 MnO 3.07 Ò 3.9098 3.9352 — 60.15 La 0.5 Bi 0.5 MnO 3.04 Î 5.5456 5.5879 7.7862 61.095 La 0.5 Bi 0.5 MnO 2.99 �O 5.501 5.8266 7.6635 61.41 magnets with weak cooperative exchange interac- tions. Ferromagnetic solutions (x � 0 4. ) are soft magnetic materials whereas in samples with x � 0 5. the coercive force sharply increases. The tempera- ture curves of the magnetization obtained in a rather small external magnetic field of 100 Oe are shown in Fig. 2. The measurements were performed in a mode of heating after cooling in a field (FC) and without a field (ZFC). It follows from the dia- grams that the Curie temperature decreases with in- crease of bismuth content. The ZFC magnetization of a sample with x � 0.6 has a wide maximum, which is typical for a magnet near the concentra- tion transition from a ferromagnetic state to the state such as a spin glass. On further increase of the bismuth content the magnetic susceptibility sharply decreases. The ZFC magnetization in a sample with x � 0.65 has a well-defined maximum. Near the temperature of the maximum the ZFC and FC magnetizations diverge. Taking into account the form of M(Í) curve we believe that in solutions with x � 0.65 the long-range magnetic order is ap- parently destroyed. The compound La0.5Bi0.5MnO3.07 was reduced under various conditions. As a result, two com- pounds — La0.5Bi0.5MnO3.04 and La0.5Bi0.5MnO2.99 are obtained. The partially reduced sample had an O-orthorhombically distorted unit cell (a c b� �2 ), whereas the strongly reduced had O�-orthorhom- bically deformed unit cell (c a b2 � � ). It should be noted, that O�-orthorhombic distortions in man- ganites indicate orbital ordering [17]. The field curves of the magnetization at liquid helium tem- perature for reduced samples are plotted in Fig. 3. The magnetizations of compounds with � = 0.04 and � = 0.07 differ slightly, whereas the composi- tion with � = – 0.01 has a very small spontaneous magnetization (about 0.2 B in formula units). With loss of oxygen the critical temperature at which a spontaneous magnetization appears at first decreased and then increased again and, moreover, the transition to the paramagnetic state became sharper (Fig. 4). It should be noted that with decrease of the oxy- gen content in the reduced manganites the mag- netic anisotropy increased sharply. Compounds with stoichiometric oxygen (x � 0.65) are hard, strongly anisotropic magnets. The coercive force HC at helium temperature reaches 15 kOe, where- as for the ferromagnetic oxidized compositions HC = 100 Oe. As compounds with bismuth content above 65% may not be obtained in air, synthesis of solutions in the range 0.7 � �x 1 is performed at high pressures. We have found out that the Curie temperature in- creases smoothly with increase of bismuth content from 87 K (x � 0.65) up to 108 K for BiMnO3. The spontaneous magnetization grows sharply on going from a solution with x � 0.8 to a solution with x � 0.9. It is necessary to note that the growth of the spontaneous magnetization correlates with a change of the unit cell symmetry type from ortho- rhombic (x � 0.8) to monoclinic (x � 0.9). Measurements of the electrical conductivity are carried out in a temperature range of 77–350 K. All of the compounds under study had a semiconductor character of the temperature dependence of the electrical resistance. Near the temperature of mag- netic ordering for structures with x � 0.4 a maxi- mum of the magnetoresistance was observed (up to 40% in a field 9 kOe), but magnetic ordering did not change the type of the conductivity. Figure 5 presents the magnetic phase diagram of the La1–xBixMnO3,07 system with an excess of oxy- gen. The ferromagnetic state is gradually destroyed with increase of the bismuth content, until in the Fizika Nizkikh Temperatur, 2002, v. 28, No. 7 793 Magnetic phase transitions in the system La1–x Bi x MnO3+� Fig. 5. Magnetic phase diagram of the La1-xBixMnO3.07 system. P – paramagnetic state, F – ferromagnetic, SG – spin glass. Fig. 6. Magnetic phase diagram of the La1–xBixMnO3 system. WF — weak ferromagnetic state, Ð — paramagnetic, F — ferromagnetic. solution with x � 0.65 the state of the cluster-type spin glass is not stabilized. The magnetic phase diagram of the stoichio- metric structures La1-xBixMnO3 is shown in Fig. 6. LnMnO3 is a weak ferromagnet with Néel tempera- ture TN � 144 K. With increase of the bismuth con- tent up to x � 0.65 the stoichiometric structures still show the properties inherent to a weak ferro- magnet. The Néel temperature gradually decreases to 87 K (x � 0.65), apparently is because of a de- crease of the Mn–O–Mn bond angles. The lower the Mn–O–Mn angle, the lower are the width of the 3d band and the temperature of magnetic order- ing [18–21]. It is well known that in LaMnO3 antiferrodistortion ordering of the dz2 orbitals oc- curs in the ab plane as the exchange interaction be- comes ferromagnetic in this plane and antifer- romagnetic along the c axis [18]. The magnetic moments are oriented along the b axis. In Bi-substi- tuted stoichiometric manganites (õ 0.6) another type of antiferromagnetic and orbital ordering is in principle possible. However, in order to ascertain the features of the magnetic and structural state, neutron diffraction studies are required. In bismuth manganite the orbital state dx y2 2� is stabilized, leading to an isotropic ferromagnetic state [14,21]. BiMnO3 is a soft magnetic material, despite the or- bital ordering [14,22]. In solutions with a high bis- muth content the magnetic state is most likely a two-phase one. The sample consists of ferromag- netic and antiferromagnetic areas. We believe that each type of magnetic state is characterized by its own type of orbital state. It is well known that in manganites the substitu- tion of the rare-earth ions R3+ and La3+ by an alka- line-earth ion results in orbital disordering and sta- bilization of the ferromagnetic state. This process is caused by two factors. First, vacancies appear in the orbitally ordered lattice (not Jahn–Teller ions Mn4+), and that destabilizes a cooperative orbital ordering. Second, distortions of the crystal lattice decrease due to optimization of the cation’s sizes, whereas the Mn–O–Mn bond angle which descri- bes the width of the 3d band, is increased. Under these conditions the static Jahn–Teller distortions transform to dynamic ones, and the exchange inter- actions of the Mn3+–O–Mn3+ and Mn3+–O–Mn4+ types become ferromagnetic [18]. The establish- ment of magnetic order in structures with a large enough width of the 3d band leads to transition in metallic state due to overlapping of the bands formed mainly by 3d and 2ð states. In manganites containing a large quantity of Bi3+ ions the appearance of tetravalent ions of man- ganese does not induce ferromagnetism (Fig. 3). The presence of Mn4+ ions promotes the destruction of cooperative orbital ordering and the occurrence of properties inherent to spin glasses. Thus the compounds remain insulators. We believe that in compounds with a large content of Bi3+ ions the lo- cal static Jahn–Teller distortions are not removed. This is explained by the tendency of Bi3+ ions to form strongly anisotropic covalent ps bonds. These bonds promote local crystal structure distortions, which is the reason why the local Jahn–Teller or- bital ordering is preserved. Indeed, the tempera- ture of the charge and orbital ordering in Bi0.5Sr0.5MnO3 is unusually high, above 500 K [23,24], whereas the characteristic temperature of charge and orbital ordering in the structures R0.5Sr0.5MnO3 is 150 K [25,26]. Due to the local static Jahn–Teller distortions, the anisotropic cha- racter of the exchange interactions between the manganese ions persist. On the other hand, in these samples, due to fluctuations of the composi- tion, microareas may exist in which the static Jahn–Teller distortions are removed. These micro- areas are ferromagnetic. The competition between ferromagnetism and antiferromagnetism results in a spin glass state of a cluster type. It should be noted that orbital and charge ordering in manganites are transitions of the martensitic type [27,28]. There- fore orbitally two-phase states in manganites should be realized at the concentration and tempe- rature boundaries of the orbital order–disorder transitions. Summary The crystal structure and magnetic properties of both oxidized La1-xBixMnO3.07 and reduced La1-xBixMnO3 perovskites have been studied. It is shown that oxidized La1-xBixMnO3.07 series exhibit a concentration transition from ferromagnetic state to spin glass at x � 0.65 whereas reduced La1-xBixMnO3 perovskites transform from weak ferrimagnet state to ferromagnetic one at x � 0.7 through a mixed magnetic state. The results obtained are discussed in terms of interplay between orbital ordering and type of magnetic ground state. 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