Antiferromagnet–ferromagnet transition in the cobaltites

The three series oxygen-deficient cobaltites La₀.₅Ba₀.₅CoO₃₋δ, LnBaCo₂O₅.₅ and Sr₂YCo₄O₁₀.₅ have been studied. It has been shown that La₀.₅Ba₀.₅CoO₃ is an insulating ferromagnet whereas La₀.₅Ba₀.₅CoO₂.₇₅ is a pure antiferromagnet in which the oxygen vacancies are disordered. The oxygen-vacancies o...

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Дата:2012
Автори: Troyanchuk, I.O., Bushinsky, M.V., Karpinsky, D.V., Sirenko, V.A.
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Опубліковано: Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України 2012
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Цитувати:Antiferromagnet–ferromagnet transition in the cobaltites / I.O. Troyanchuk, M.V. Bushinsky, D.V. Karpinsky // Физика низких температур. — 2012. — Т. 38, № 7. — С. 833-841. — Бібліогр.: 53 назв. — англ.

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Digital Library of Periodicals of National Academy of Sciences of Ukraine
id nasplib_isofts_kiev_ua-123456789-117271
record_format dspace
spelling Troyanchuk, I.O.
Bushinsky, M.V.
Karpinsky, D.V.
Sirenko, V.A.
2017-05-21T17:19:48Z
2017-05-21T17:19:48Z
2012
Antiferromagnet–ferromagnet transition in the cobaltites / I.O. Troyanchuk, M.V. Bushinsky, D.V. Karpinsky // Физика низких температур. — 2012. — Т. 38, № 7. — С. 833-841. — Бібліогр.: 53 назв. — англ.
0132-6414
PACS: 75.50.Dd, 75.30.–m, 75.60.Ej
https://nasplib.isofts.kiev.ua/handle/123456789/117271
The three series oxygen-deficient cobaltites La₀.₅Ba₀.₅CoO₃₋δ, LnBaCo₂O₅.₅ and Sr₂YCo₄O₁₀.₅ have been studied. It has been shown that La₀.₅Ba₀.₅CoO₃ is an insulating ferromagnet whereas La₀.₅Ba₀.₅CoO₂.₇₅ is a pure antiferromagnet in which the oxygen vacancies are disordered. The oxygen-vacancies ordering leads to appearance of the ferromagnetic component apparently due to a formation of the noncollinear magnetic structure. The antiferromagnet–“ferromagnet” transition is accompanied by a giant magnetoresistance. It is suggested that in the ferromagnetic oxidized compounds Co³⁺ and Co⁴⁺ ions adopt intermediate spin state whereas for antiferromagnetic (Co⁴⁺-free) compositions Co³⁺ ions have high-spin state (pyramids CoO₅) and dominant low-spin state (octahedra CoO₆). In both ferromagnetic and antiferromagnetic compounds the superexchange via oxygen plays an essential role in a formation of the magnetic properties.
The authors would like to acknowledge the financial support of the BRFFI (Grant Nos. T11D-003).
en
Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України
Физика низких температур
Магнетизм
Antiferromagnet–ferromagnet transition in the cobaltites
Article
published earlier
institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
collection DSpace DC
title Antiferromagnet–ferromagnet transition in the cobaltites
spellingShingle Antiferromagnet–ferromagnet transition in the cobaltites
Troyanchuk, I.O.
Bushinsky, M.V.
Karpinsky, D.V.
Sirenko, V.A.
Магнетизм
title_short Antiferromagnet–ferromagnet transition in the cobaltites
title_full Antiferromagnet–ferromagnet transition in the cobaltites
title_fullStr Antiferromagnet–ferromagnet transition in the cobaltites
title_full_unstemmed Antiferromagnet–ferromagnet transition in the cobaltites
title_sort antiferromagnet–ferromagnet transition in the cobaltites
author Troyanchuk, I.O.
Bushinsky, M.V.
Karpinsky, D.V.
Sirenko, V.A.
author_facet Troyanchuk, I.O.
Bushinsky, M.V.
Karpinsky, D.V.
Sirenko, V.A.
topic Магнетизм
topic_facet Магнетизм
publishDate 2012
language English
container_title Физика низких температур
publisher Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України
format Article
description The three series oxygen-deficient cobaltites La₀.₅Ba₀.₅CoO₃₋δ, LnBaCo₂O₅.₅ and Sr₂YCo₄O₁₀.₅ have been studied. It has been shown that La₀.₅Ba₀.₅CoO₃ is an insulating ferromagnet whereas La₀.₅Ba₀.₅CoO₂.₇₅ is a pure antiferromagnet in which the oxygen vacancies are disordered. The oxygen-vacancies ordering leads to appearance of the ferromagnetic component apparently due to a formation of the noncollinear magnetic structure. The antiferromagnet–“ferromagnet” transition is accompanied by a giant magnetoresistance. It is suggested that in the ferromagnetic oxidized compounds Co³⁺ and Co⁴⁺ ions adopt intermediate spin state whereas for antiferromagnetic (Co⁴⁺-free) compositions Co³⁺ ions have high-spin state (pyramids CoO₅) and dominant low-spin state (octahedra CoO₆). In both ferromagnetic and antiferromagnetic compounds the superexchange via oxygen plays an essential role in a formation of the magnetic properties.
issn 0132-6414
url https://nasplib.isofts.kiev.ua/handle/123456789/117271
citation_txt Antiferromagnet–ferromagnet transition in the cobaltites / I.O. Troyanchuk, M.V. Bushinsky, D.V. Karpinsky // Физика низких температур. — 2012. — Т. 38, № 7. — С. 833-841. — Бібліогр.: 53 назв. — англ.
work_keys_str_mv AT troyanchukio antiferromagnetferromagnettransitioninthecobaltites
AT bushinskymv antiferromagnetferromagnettransitioninthecobaltites
AT karpinskydv antiferromagnetferromagnettransitioninthecobaltites
AT sirenkova antiferromagnetferromagnettransitioninthecobaltites
first_indexed 2025-11-24T20:17:21Z
last_indexed 2025-11-24T20:17:21Z
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fulltext © I.O. Troyanchuk, M.V. Bushinsky, D.V. Karpinsky, and V.A. Sirenko, 2012 Low Temperature Physics/Fizika Nizkikh Temperatur, 2012, v. 38, No. 7, pp. 833–841 Antiferromagnet–ferromagnet transition in the cobaltites I.O. Troyanchuk, M.V. Bushinsky, and D.V. Karpinsky Scientific-Practical Materials Research Centre of NAS of Belarus 19 P. Brovka Str., Minsk 220072, Belarus V.A. Sirenko B. Verkin Institute for Low Temperature Physics and Engineering of the National Academy of Sciences of Ukraine 47 Lenin Ave., Kharkov 61103, Ukraine E-mail: sirenko@ilt.kharkov.ua Received March 13, 2012 The three series oxygen-deficient cobaltites La0.5Ba0.5CoO3–δ, LnBaCo2O5.5 and Sr2YCo4O10.5 have been studied. It has been shown that La0.5Ba0.5CoO3 is an insulating ferromagnet whereas La0.5Ba0.5CoO2.75 is a pure antiferromagnet in which the oxygen vacancies are disordered. The oxygen-vacancies ordering leads to appear- ance of the ferromagnetic component apparently due to a formation of the noncollinear magnetic structure. The antiferromagnet–“ferromagnet” transition is accompanied by a giant magnetoresistance. It is suggested that in the ferromagnetic oxidized compounds Co3+ and Co4+ ions adopt intermediate spin state whereas for antiferro- magnetic (Co4+-free) compositions Co3+ ions have high-spin state (pyramids CoO5) and dominant low-spin state (octahedra CoO6). In both ferromagnetic and antiferromagnetic compounds the superexchange via oxygen plays an essential role in a formation of the magnetic properties. PACS: 75.50.Dd Nonmetallic ferromagnetic materials; 75.30.–m Intrinsic properties of magnetically ordered materials; 75.60.Ej Magnetization curves, hysteresis, Barkhausen and related effects. Keywords: antiferromagnet, oxygen vacancies, spin state transition, layered perovskite. 1. Ferromagnetic and antiferromagnetic phases in the anion deficient cobaltites with disordered oxygen vacancies Rare earth cobaltites Ln1–xAxCoO3 (Ln = lanthanide, A = alkaline earth metal: Ca, Sr or Ba) with perovskite structure attract much interest as they exhibit a variety of unusual magnetic and transport properties [1–5]. The Co ions in octahedral symmetry may have either high, inter- mediate or low-spin state as the energies of the crystalfield splitting of both the Co 3d states and the Hund’s rule ex- change energy are comparable. In the ground state at low temperature, LaCoO3 contains Co3+ ions with the low-spin electronic configuration 6 0 2g gt e [1–3]. Upon heating, the spin state of Co ions thermally activates to the intermediate state (IS, 5 1 2g gt e , S = 1) or high-spin state (HS, 4 2 2g gt e , S = 2) [1–3]. In the hole-doped cobaltites, La1–xAxCoO3, the addi- tional Co4+ ion increases the complexity of the system as it can also be in the different spin states. Among doped cobaltites, the system La1–xSrxCoO3 is the most extensive- ly investigated. A spin glass behavior was reported for x < 0.18 as well as a ferromagnetic long-range ordering that coincides with concentration insulator-to-metal transi- tion for x ≈ 0.18 [6]. Similar metallic ferromagnetic state was observed in barium-doped cobaltites with barium con- tent x > 0.2 [7–9]. The structural studies performed on the cubic oxygen-stoichiometric perovskite La0.5Ba0.5CoO3 have revealed an onset of a long-range tetragonal phase accompanying a para-ferromagnetic transition at TC ≈ 180 K [10,11]. The tetragonal distortion has been discussed in terms of cooperative Jahn–Teller distortions of the CoO6 octahedra. It was assumed that the Jahn–Teller effect is favored by the intermediate spin-state configura- tion of the Co3+(d6) and Co4+(d5) ions derived from the measured ferromagnetic moment –1.9 μB per cobalt ion. However, the Sr-doped ferromagnetic cobaltites have ap- proximately the same magnetic moment value and do not exhibit any structural transition at the Curie point [12,13]. Moreover the extended x-ray absorption fine structure (EXAFS) and neutron diffraction studies do not reveal any appreciable local Jahn–Teller distortion in La1–xSrxCoO3 [14]. The nature of the ferromagnetic state in cobaltites was a subject of debates for a long time [15–17]. Three main I.O. Troyanchuk, M.V. Bushinsky, D.V. Karpinsky, and V.A. Sirenko 834 Low Temperature Physics/Fizika Nizkikh Temperatur, 2012, v. 38, No. 7 mechanisms explaining magnetic properties of mixed-va- lence cobaltites were suggested: the superexchange model based on the localized electron interaction via oxygen ion, the Zener double exchange via charge transfer and the itin- erant electron ferromagnetism [15–17]. Besides the alkaline earth doping there is another way to manipulate the physical properties of the rare earth cobaltites. In accordance with [18,19] the oxygen deficien- cy in La0.5A0.5CoO3–δ (A = Sr, Ba) perovskites is accom- panied by a strong decrease of magnetization and phase separation phenomenon. The crystal structure of the La0.5Ba0.5CoO3–δ has been analyzed using x-ray, neutron and synchrotron diffraction techniques. The XRD data obtained at room temperature verify the cubic structure of the La0.5Ba0.5CoO3–δ up to concentration x = 0.45. The neutron diffraction data for the La0.5Ba0.5CoO3–δ sample cooled at a rate of 300 °C/h from 1200 °C have been rec- orded at temperatures of 300, 150, 80 and 2 K. Rietveld refinement performed for the 300 K NPD pattern assumes cubic symmetry of the compound ( 3Pm m space group). The structural analysis performed by using the tetragonal space group (P4/mmm), rhombohedral ( 3R c), and ortho- rhombic one (Pnma) did not result in any essential im- provement of the reliability factors and cubic structure has been assumed as a more feasible one. The value of the oxy- gen occupation refined from the NPD data at 300 K is about 2.88, the cubic symmetry supposes a random distri- bution of the oxygen vacancies as well as of La and Ba ions. The crystal structure has been additionally studied by using synchrotron powder diffraction. In order to estimate the structural parameters in detail, the SPD patterns were recorded in the range from 5 K up to 300 K at the 5 K step. The refinement of the SPD pattern recorded at 300 K, has confirmed the macroscopic cubic symmetry ( 3 )Pm m of the La0.5Ba0.5CoO2.88. However, close inspection of the SPD patterns has revealed a very small asymmetric broadening of the diffraction peaks. The asymmetry becomes more pronounced with temperature decreasing. Similar behavior of the NPD and SPD diffraction peaks excludes possible instrumental faults and/or texturing effects that could lead to an asymmetry of the peaks. Analysis of the NPD and SPD patterns recorded at temperatures below 150 K clari- fies a cause of the phase instability. The most probable reason for the peak asymmetry is an appearance of a new phase with structural parameters larger than those for the parent phase. The diffraction patterns recorded at low tem- peratures have uniquely confirmed the phase separation scenario (Fig. 1). The structure refinement using two-phase model with cubic unit cells for the diffraction patterns ob- tained for T < 150 K, strongly improves the reliability fac- tors. The refined structural data have confirmed gradual extension of the new cubic phase with temperature de- crease. The content of the phase with the smaller lattice parameter calculated from the refinement of the NPD pat- tern recorded at 2 K, is about 70% (the major phase). The rough estimation of the oxygen content performed for the NPD data taken at 2 K, assumes the oxygen content for the phase with the larger lattice parameter to be smaller as compared with the major structural phase. However, the overlapping of the diffraction peaks hampers an accurate determination of the oxygen content for the both structural phases. The difference in the oxygen content assumes a slightly different oxidation state and coordination for Co ions in these phases. One can suggest that in the minor phase Co ions have the oxidation state close to 3+ and are located in the oxygen pyramids and octahedra whereas in the major phase the cobalt ions are placed predominantly in the oxygen octahedra and have a mixed 3+/4+ oxidation state. It should be noted that stoichiometric La0.5Ba0.5CoO3 is a single phase down to the liquid heli- um temperature [10,11]. So, the oxygen deficit is the im- portant factor in the phase separation. The NPD data permit to clarify the magnetic structure of the La0.5Ba0.5CoO2.88. Taking into account the SPD data for La0.5Ba0.5CoO2.88 the additional peaks occurring only on NPD patterns below 150 K can be referred to magnetic neutron scattering. The NPD patterns were well fitted assuming the coexistence of ferromagnetic and G- type antiferromagnetic structures. An additional contribu- tion to the intensities of the diffraction peaks (100), (110), (210) testifies long range ferromagnetism within the com- pound, whereas the new magnetic peaks indexed as (111), (113), (313) in 2ap×2ap×2ap cubic metric assume antifer- romagnetic ordering. Based on the structural data the fer- romagnetic contribution is attributed to the major structural phase, whereas G-type antiferromagnetic one is associated with the minor phase with larger unit cell. The estimated magnetic moments are approximately ~1.6 μB for F-type phase and ~2 μB for G-type antiferromagnetic phase. The Fig. 1. The synchrotron diffraction spectra for the La0.5Ba0.5CoO3–δ compound at 4 K. The observed and calculated profiles are noted by points and the line, respectively, the bottom line represents their difference. The data are refined in 3Pm m space group for the both structural phases. The inset shows the magnified parts of the patterns at 300 K. 5 15 25 35 45 0 20 40 60 80 100 In te ns ity , a rb . u ni ts In te ns ity , a rb . u ni ts 2 , degθ 2 , degθ T = 4 K 31.0 31.5 32.0 32.5 33.0 300 K T = 4 K Antiferromagnet–ferromagnet transition in the cobaltites Low Temperature Physics/Fizika Nizkikh Temperatur, 2012, v. 38, No. 7 835 calculated moment for the ferromagnetic phase correlates with the published data for the oxygen stoichiometric La and Ba ordered LaBaCo2O6 (1.5 μB) and disordered La0.5Ba0.5CoO3 (1.9 μB) ferromagnetic phases [10,11]. The La0.5Ba0.5CoO2.77 sample reveal exceptional be- havior of the unit cell parameter with temperature change. The unit cell parameter decreases with temperature reduc- tion from room temperature down to ~170 K where pure antiferromagnetic order develops. Whereas below the tem- perature of antiferromagnetic ordering an unexpected gradual increase of the lattice parameter is observed. The unit cell volume estimated for the La0.5Ba0.5CoO2.77 com- pound at 2 K is close to that observed at room temperature. The phase separation phenomena as well as ferromagnetic contribution into NPD pattern have not been observed. We suggest that the most probable reason of the unusu- al expansion of the unit cell as well as phase separation is transition of the Co3+ ions to the high/low-spin state from initially an intermediate spin state which is more stable at high temperature. The structural phase separation can be accompanied by redistribution of the electronic density (electronic phase separation). The magnetization data seem to be in agreement with this assumption. The oxidized La0.5Ba0.5CoO3–δ being cooled slowly from 1200 °C shows magnetic moment about 1.8 μB corresponding to the intermediate spin state of the Co3+/Co4+ ions for pure fer- romagnetic state. Decreasing of the oxygen content lead to drop of the magnetic moment and anomalous magnetiza- tion behavior thus indicating the spin-state transition (Fig. 2). The pure antiferromagnetic compositions do not show remnant magnetization. In accordance with [20] we suggest that high-spin state is stabilized in pyramids whereas low-spin state corresponds to octahedra. A relatively large negative magnetoresistance is ob- served in nearly stoichiometric oxidized La0.5Ba0.5CoO3–δ. Figure 3 shows the temperature variations of electrical re- sistivity measured at different external magnetic fields for La0.5Sr0.5CoO3–δ (upper panel) and La0.5Ba0.5CoO3–δ (lo- wer panel). Both the samples are pure ferromagnets. The resistivity of La0.5Sr0.5CoO3–δ exhibits the metallic behav- ior within the whole measured temperature range from 5 to 300 K. The nonpronounced anomaly in the ρ(T) depend- ence was observed near the Curie point at the absence of the external magnetic field. The magnetoresistance is not revealed at low temperatures but appeared around TC, as is shown in Fig. 3. The temperature variation of resistivity for La0.5Ba0.5CoO3–δ is dramatically different. The metallic behavior of the resistivity has been observed only in the narrow temperature range near the Curie point TC ~ 170 K, and it gradually changes to a semiconducting one below 150 K. An external magnetic field strongly extends the metallic-like temperature range above the Curie point, however at low temperatures the semiconductive behavior does not essentially change. Figure 4 shows magnetoresis- tance as a function of a field at various temperatures for La0.5Ba0.5CoO3–δ. The magnetoresistance exhibits a local maximum near the TC and increases gradually with further cooling. At 5 K we obtained the MR value of about 20% in the field of 14 T. The MR varies gradually with the field and does not show any tendency to saturation with the temperature decrease. Fig. 2. The magnetization vs temperature dependencies of the La0.5Ba0.5CoO3–δ quenched from 750 and 650 °C. The arrows indicate temperature change direction. 0 50 100 150 200 250 3000.1 0.4 0.7 1.0 1.3 1.6 1.9 750 °C H = 1 T La Ba CoO0.5 0.5 3–δ Tq = 650 °C M , e m u/ g T, K Fig. 3. The resistivity of ferromagnetic La0.5Sr0.5CoO3–δ (top panel) and La0.5Ba0.5CoO3–δ (bottom panel) cooled at a rate of 100 °C/h vs temperature. The inset shows the resistivity behavior near the Curie point. 0 50 100 150 200 250 300 9.0 7.5 6.0 4.5 3.0 2.5 2.0 1.5 1.0 0.5 T, K T, K 120 140 160 180 200 220 10 T 5 T 3.4 3.5 3.6 3.7 3.8 0 T 14 T H = 0 ρ Ω , ·c m 10 –3 ρ Ω , ·c m 10 –3 ρ Ω , ·c m 10 –4 I.O. Troyanchuk, M.V. Bushinsky, D.V. Karpinsky, and V.A. Sirenko 836 Low Temperature Physics/Fizika Nizkikh Temperatur, 2012, v. 38, No. 7 There are different types of the large magnetoresistance ratio observed in the ordinary cobaltites. The large magne- toresistance was observed in the insulating spin-glass pha- se of the lightly doped La1–xSrxCoO3 cobaltites [21,22]. It is suggested that the interface effects associated with diffe- rent magnetic and conductive states of ferromagnetic clus- ters and paramagnetic matrix are responsible for nonsatu- rated magnetoresistance observed in the large magnetic field [21]. This type of magnetoresistance is the most pro- nounced at low temperature. The second type of large magnetoresistance was observed at the low temperature in the insulating homogeneous ferromagnet La0.5Ba0.5CoO3 [10,11]. This type of magnetoresistance has similar tem- perature and field dependences with magnetotransport pa- rameters of the lightly doped cobaltites. The magnetoresis- tance is not saturated in the large magnetic field and strongly increases while temperature decreasing. In con- trast to manganites there is no large magnetotransport anomaly in the vicinity of the Curie point. The observation of the homogeneous ferromagnetism in insulating La0.5Ba0.5CoO3 in our opinion, confirms the hypothesis that ferromagnetic properties of the hole-doped cobaltites with the perovskite structure are governed by the superexchange interactions similar to those in oxides of the nonmixed valence type of magnetoactive ions (e.g., ferrites with Fe3+ ions). The small magnetotransport and conduc- tivity anomalies near the Curie point of the both insulating and conductive cobaltites apparently do not support the dominant role of the “double exchange” in defining of the ferromagnetic ordering as it was suggested in a number of works [6,10,11]. The insulating character of the La0.5Ba0.5CoO3 ferromagnetic phase cannot be understood by means of the “itinerant magnetism” model. Apparently large magnetoresistance observed in homogeneous La0.5Ba0.5CoO3 at low temperature is associated with de- creasing of the insulating gap between eg and collective t2g state upon external magnetic field. 2. Antiferromagnet–ferromagnet transition in iron doped TbBaCo2O5.5 layered perovskite The layered perovskites LnBaCo2O5.5 (Ln = lanthanide) have attracted a great attention due to interplay between magnetic and magnetotransport properties [23–26]. The crystal structure of these compounds has an alternating linkage of Ba2+ and Ln3+ layers along the c axis and layers of CoO5 pyramids and CoO6 octahedrons along the a or b axis [25]. As a result of ordering of Ln3+ and Ba2+ ions as well of oxygen vacancies the crystal structure is described with unit cell ap×2ap×2ap in the space group Pmmm. The LnBaCo2O5.5 compounds exhibit following tran- sitions: antiferromagnet–“ferromagnet” in the temperature range 200 K ≤ T < 260 K, “ferromagnet”–paramagnet (250 K < T < 300 K) and metal–insulator (300 K < T < 370 K) depending on Ln ion size [23–25]. According to the neu- tron diffraction studies the “ferromagnetic” phase consists of the basic G-type antiferromagnetic (2ap×2ap×2ap) and small ferromagnetic components, while the low- temperature pure antiferromagnetic phase has magnetic unit cell of 2ap×2ap×4ap-type [27–30]. The transition antiferromagnet–“ferromagnet” leads to a drop of the resis- tivity and a giant magnetoresistance effect [23–26]. The reason for interplay between magnetic and magnetotransport properties is not clear so far. In order to understand magnetotransport properties the detailed de- scription of the magnetic structure in the both phases is necessary. Several studies of magnetic structure of the LnBaCo2O5.5 compounds have been performed with di- verging results [27–34]. According to [30,34] the magnetic structure is noncollinear in both antiferromagnetic and fer- romagnetic phases. The Co3+ ions in octahedrons adopt the low-spin state [30,34], whereas in pyramids they are in the high-spin state. In works [27,28] it was suggested that the correct space group is Pmma and the crystal structure is described with a 2ap×2ap×2ap supercell. In this model Co3+ ions in both pyramidal and octahedral sublattices are located in nonequivalent two sites and magnetic structure can be described by a collinear model for both “ferromag- netic” and antiferromagnetic phases. It worth to be noted that symmetry analysis performed for both space groups Pmmm and Pmma does not allow realization of the noncol- linear magnetic structure with ferromagnetic component. However, a synchrotron x-ray powder diffraction study of YBaCo2O5.5 compound has revealed some additional peaks associated with a 2ap×2ap×2ap crystal structure supercell and small monoclinic distortion in the ferromag- netic phase corresponding space group P112/a [35]. The observed monoclinic distortion support the model of the noncollinear magnetic structure for description of magnetic and magnetotransport properties of LnBaCo2O5.5-type compounds. Very intricate properties have been revealed in TbBaCo2O5.5–x/2 doped with Fe3+ ions [26,36]. In Fig. 4. Field dependencies of the magnetoresistance ratio MR = [ρ(H) – ρ(H = 0)]/ρ(H = 0)·100% for the ferromagnetic La0.5Ba0.5CoO3–δ. 0 2 4 6 8 10 12 14–20 –15 –10 –5 0 H, T 100 K 170 K 50 K 5 K 15 K M R , % Antiferromagnet–ferromagnet transition in the cobaltites Low Temperature Physics/Fizika Nizkikh Temperatur, 2012, v. 38, No. 7 837 TbBaCo2–xFexO5.5 below x = 0.1 orthorhombic distortion slightly increases with increasing Fe3+ content and disap- pears above x = 0.15. The temperature of “ferromagnet”–pa- ramagnet transition increases while the temperature of “ferromagnet”–antiferromagnet transition decreases with increasing Fe3+ content up to x = 0.1. Transition into te- tragonal phase (x > 0.15) leads to a collapse of the ferro- magnetic phase. The jump of conductivity as well as ther- mal hysteresis associated with “ferromagnet”–antiferro- magnet transition become much larger with Fe doping within orthorhombic phase. The antiferromagnetic phase becomes proof against external magnetic field. Mössbauer study has revealed that Fe3+ ions predominantly occupy two strongly distorted positions [36]. The results of measurements of ZFC and FC magnetization of TbBaCo1.9Fe0.1O5.5 used for neutron diffraction are shown in Fig. 5. Both ZFC and FC magnetizations exhibit a sharp maxima at T = 300 K which indicate the transition into a paramagnetic state. In the temperature interval 200–170 K the field cooled mag- netization decreases strongly with lowering temperature. In this temperature range ZFC magnetization changes very little thus indicating a huge magnetic anisotropy. It should be noted that ZFC and FC magnetizations do not coincide below 170 K down to liquid helium temperature due to a presence of a small remnant magnetization. The good ag- reement between calculated and observed profiles of NPD patterns was reached using Pmmm space group with a 2ap×ap×2ap unit cell. The refinement in Pmma space group with 2ap×2ap×2ap unit cell leads to the same factors of reliability as refinement in terms of Pmmm model. Analysis of the powder patterns collected at the temper- ature 215 K shows that there is a set of the additional mag- netic reflections which could be indexed using a 2ap×2ap×2ap magnetic unit cell. Furthermore the addition- al contribution into (100) reflection has been clearly ob- served. This contribution disappears at 130 K. The contri- bution into reflection (100) corresponds to the ferromag- netic component whereas the appearance of (111), (311), (113), (331) and (313) reflections corresponds to the G- type antiferromagnetic component. The contribution into the G-type antiferromagnetic component increases with decreasing temperature down to 130 K whereas the ferro- magnetic contribution disappears. Such a type of behavior of the antiferromagnetic component was observed first for the LnBaCo2O5.5-type layered perovskites exhibiting antiferromagnet–“ferromagnet” transition. The low-tempe- rature antiferromagnetic phase of the undoped compounds is described with a more complex 2ap×2ap×4ap magnetic unit cell [27–32]. The refinement of the magnetic structure at 215 K gives following values of magnetic moments for the G-type antiferromagnetic component: 1.9 μB per Co ion for the pyramidal sublattice and 0.9 μB for the octahe- dral one. The ferromagnetic component is 1.0 μB per for- mula unit and directed along the b axis, whereas the anti- ferromagnetic component is along the a axis. All the magnetic moments are placed within (a,b) plane. Decreas- ing temperature down to 130 K leads to increasing magnet- ic moment up to 2.6 μB for the pyramidal sublattice while for octahedral one it practically does not change. The magnetic moment value in the pyramidal sublattice is 2.6 μB per ion at 130 K. This value is significantly more than 2 μB associated with the intermediate spin state. It was found that magnetic moments of the high-spin Co3+ ions in Sr2Co2O5 and BiCoO3 are 3.3 and 3.4 μB, respectively [37,38]. However, the magnetic moment of the Co3+ ion in high-spin state (S = 2) should be about 4 μB. So, present data can hardly be adjusted with a pure ionic model for Co ions magnetic moments. In Refs. 2, 3 the Co3+ ions in LaCoO3 have been shown to have first excited state corresponding to the high-spin one. Probably it is valid for LnBaCo2O5.5-type compounds. Hence, the description of the magnetic state of Co3+ ions in TbBaCo2O5.5 doped with iron could be done in terms of a mixed low/high-spin magnetic state. The results of NMR study of EuBaCo2O5.5 are in agreement with a mixed low-high spin state model [39]. Both “ferromagnetic” and antiferromagnetic phases in TbBaCo1.9Fe0.1O5.5 have the G-type magnetic structure with a 2ap×2ap×2ap magnetic unit cell. In this magnetic structure there are only two different magnetic positions for both CoO5 and CoO6 layers. The transition into the antiferromagnetic phase leads to a substantial increase of magnetic moments in pyramidal sublattice, whereas mag- netic moments in the octahedrons remain practically the same. These results can be easily understood in noncolline- ar model of the magnetic structure of the “ferromagnetic” phase. Apparently in the ferromagnetic phase an angle be- tween magnetic moments of the Co3+ ions in pyramidal sublattice in direction of the a axis is about 30°. In the anti- ferromagnetic phase the magnetic structure seems to be collinear and aligned along the b axis because the 2ap×2ap×2ap magnetic unit cell is preserved. Remind, that in the undoped TbBaCo2O5.5 the low-temperature antifer- Fig. 5. The temperature dependences of the magnetization for TbBaCo1.9Fe0.1O5+γ measured in the FC and ZFC modes at H = 0.05 T. 0 100 200 300 0 0.6 1.2 , KT M , e m u/ g H = 0.05 T FC ZFC TbBaCo Fe O1.9 0.1 5+γ I.O. Troyanchuk, M.V. Bushinsky, D.V. Karpinsky, and V.A. Sirenko 838 Low Temperature Physics/Fizika Nizkikh Temperatur, 2012, v. 38, No. 7 romagnetic phase remains noncollinear and the magnetic unit cell contains four sites for magnetic ions which leads to 2ap×2ap×4ap magnetic supercell [34]. In order to understand an origin of noncollinear mag- netic structure it is necessary to consider exchange interac- tions in the pyramidal sublattice. One can suppose ex- change interactions in the pyramidal sublattice to be negative in the case when nearest pyramids have common oxygen ion and positive if not. In this case all the interac- tions within (a,b) plane are negative whereas along с axis negative and positive ones are alternated. This leads to a frustration of magnetic interactions and the noncollinear magnetic structure in the some temperature range could be more favorable than the simple collinear one. The spin- orbital interaction seems to be also very important factor leading to canting of the magnetic moments. Really the measurements of magnetic and magnetotransport proper- ties performed on a single crystal have revealed a huge magnetocrystalline anisotropy as well as giant anisotropic magnetoresistance [31]. A number of noncollinear magnet- ic structures in different magnetic materials have been un- derstood in terms of itinerant magnetism approach with relativistic interactions [40]. Doping with Fe3+ stabilizes the collinear antiferromagnetic structure at low tempera- tures because all the interactions Fe3+–Fe3+, Fe3+–Co2+, Fe3+–Co3+ seem to be strongly antiferromagnetic. At high Fe doping (x > 0.1) the orthorhombic symmetry transforms to tetragonal one leading to ferromagnetic component dis- appearing [26,36]. The ferromagnetic component collapse is caused by random distribution of the octahedra and py- ramids in tetragonal phase. In the works [27,28] the noncollinear solution has been overruled on the base of symmetry analysis. However the noncollinear magnetic structures in LnBaCo2O5.5 com- pounds seem to be a result of a very small monoclinic dis- tortion whereas for symmetry analysis only orthorhombic space groups were used. The noncollinear structure is sub- tle balance between positive, negative exchange interac- tions and magnetocrystalline anisotropy. Using the conception of noncollinear magnetism one can try to explain the peculiarities of magnetic and transport properties of the layered cobaltites, associated with “ferromagnet”–antiferromagnet transition. In contrast to collinear model the noncollinear one provides pure fer- romagnetic direction orthogonal to antiferromagnetic axis. Hence the transition into noncollinear ferromagnetic phase can produce strong changes in the vicinity of Fermi level. Really in the noncollinear model antiferromagnetic com- ponent is aligned along the a axis whereas along the b axis the pure ferromagnetic component is realized thus leading to a jump of conductivity at antiferromagnet–“ferromag- net” transition. 3. Antiferromagnet–ferromagnet transition in layered Sr3YCo4O10.5+δ-type cobaltites Another class of anion-deficient layered cobaltites was received quite recently. It has the chemical composition Sr3LnCo4O10.5+δ (its reduced chemical formula is Sr0.75Ln0.25CoO3–γ), where the rare earth ions can partially substitute for strontium ions and vice versa [41–44]. Its crystal structure is built by alternating anion-deficient CoO4+δ layers and layers formed by CoO6 octahedra with sharing vertices. This class of compounds is characterized by high magnetic ordering temperature (up to 360 K) [45–47]. Spontaneous magnetization appears below 360 K, attains its maximum value near room temperature, and then decre- ases gradually down to liquid helium temperatures [45–49]. Several conjectures explaining the anomalous temperature dependence of the magnetization have been put forward. In Ref. 50, it was suggested that a certain fraction of Co3+ ions undergo the transition from the high-spin to low-spin state with a decrease in temperature. However, the neutron diffraction studies do not reveal any anomalous decrease in the magnetic moment when the temperature is decreased [48,49,51]. In the whole temperature range below the mag- netic ordering point, the antiferromagnetic G-type structure was observed, whereas it was impossible to reliably detect the ferromagnetic contribution since it turned out to be quite small. For this reason, in [48,49], the anomalous be- havior of the magnetization was attributed to the phase transition from the magnetic state with the spontaneous magnetization to the purely antiferromagnetic state. It was assumed that the transition was incomplete owing to the chemical inhomogeneity of the samples. However, another interpretation of the transition was proposed in Ref. 52, where the ferromagnetic component was determined by the neutron diffraction method. The model proposed in Ref. 52 attributes the anomalous behavior of the magnetization to the presence of a weak magnetic sublattice within the magnetic structure of the collinear ferrimagnet. In the framework of this model, the spontaneous magnetization results from the ordering of cobalt ions with different oxy- gen coordination numbers in the CoO4+δ layer, whereas the CoO6 layer is purely antiferromagnetic. According to Ref. 52, the spontaneous magnetization appears owing to the different temperature dependences of the magnetic moments of cobalt in different sublattices of the collinear ferrimagnet. The temperature dependence of the magnetization for the Sr3YCo4O10.6+δ sample obtained by fast cooling is shown in Fig. 6. The measurements were performed upon cooling and heating at different magnetic fields up to 14 T. The cooling and heating rates were 0.5 K/min. Within the temperature range of 210–240 K, a steep increase (de- crease) in the magnetization with a temperature hysteresis of 12 K has been observed. Such a temperature behavior of the magnetization is characteristic of the first-order mag- Antiferromagnet–ferromagnet transition in the cobaltites Low Temperature Physics/Fizika Nizkikh Temperatur, 2012, v. 38, No. 7 839 netic phase transition of the order–order type. In the high- temperature phase, the magnetization is not saturated at magnetic fields up to 14 T. Therefore, it is impossible to determine accurately the spontaneous magnetization. Nev- ertheless, its estimated value is no less than 0.25 μB per cobalt ion. In the temperature range corresponding to the magnetic phase transition, the magnetic field dependence of the magnetization exhibits an anomalous growth of the susceptibility at high fields and a pronounced field hystere- sis of the magnetization. Such a behavior of the magnetiza- tion is characteristic of metamagnets, i.e., materials where the applied magnetic field induces another phase state with a higher magnetization. The metamagnetic transition is incomplete since a field of 14 T is insufficient to induce a homogeneous high-temperature magnetic phase. At low temperatures (T < 150 K), the magnetic field dependence of the magnetization is almost linear, similar to that in anti- ferromagnets, whereas the spontaneous magnetization is practically absent. Both slightly reduced and oxidized sam- ples show antiferromagnet–“ferromagnet” transition also. The new results of the magnetic measurements suggest that the behavior of the magnetization for the Sr3YCo4O10.5+δ sample reported in Refs. 45–49 is associ- ated with inhomogeneous yttrium distribution over the sample. With an increase in the yttrium content, a purely ferromagnetic behavior transforms to a purely antiferro- magnetic behavior, passing through intermediate composi- tions, which exhibit the first-order antiferromagnet– “ferromagnet” phase transition (Fig. 7). It worth to be noted that the behaviors of two different classes of layered cobaltites, SrLnCo4O10.5 and LnBaCo2O5.5, are very similar. Both classes of layered cobaltites exhibit the antiferromagnet–ferromagnet transi- tion and accurately prepared polycrystalline samples have nearly the same spontaneous magnetization in the ferro- magnetic phase. This is likely due to similar mechanisms of ferromagnetism in both classes of compounds, where the antiferromagnet–ferromagnet transition can occur in the nominally G-type magnetic structure without the for- mation of additional magnetic reflections in the low- temperature antiferromagnetic phase [48,49,52,53]. This behavior can be easily explained under the assumption that the magnetic structure of the ferromagnetic phase is noncollinear with the uncompensated magnetic moment as in weak ferromagnets. The symmetry analysis forbidding the existence of noncollinear ferromagnetism in LnBaCo2O5.5 was performed within the framework of the orthorhombic Pmma space group [27]. At the same time, a careful x-ray structural analysis indicates that the true symmetry is monoclinic (P112/a) [35]. It is necessary to note that the true symmetry of Sr3YCo4O10.5+δ is also monoclinic (possible space group A2/a) [45] rather than orthorhombic, while the symmetry analysis in Ref. 52 was performed on the basis of the latter symmetry. 4. Conclusions The insulating La0.5Ba0.5CoO3 and metallic Ln0.5Sr0.5CoO3 ordinary cobaltites are ferromagnetic due to superexchange interactions via oxygen between cobalt ions in the intermediate spin state. The insulating La0.5Ba0.5CoO3 is only one known cobaltite exhibiting cooperative static Jahn–Teller distortions of the CoO6 octahedra at low temperature. The oxygen content decreas- ing leads to transformation from ferromagnetic to the G- type antiferromagnetic structure through the phase separa- ted state. The anomalous structural and magnetization be- havior apparently is associated with a spin state transition. The antiferromagnetic phase is characterized by high/low- spin state of the Co3+ ions and lack of the ferromagnetic contribution. The ordering of the oxygen vacancies in the LnBaCo2O5.5 and Sr3YCo4O10.5 layered cobaltites lead to increases of the Neel point from 170 to 380 K and appear- ance of the relatively small ferromagnetic component which is identical for both type of the layered cobaltites. Fig. 6. Temperature dependence of the magnetization for Sr3YCo4O10.5+δ samples produced upon fast cooling from 1000 °C in different magnetic fields. 50 100 150 200 250 300 1 3 5 7 9 fast cooling 7 T 14 T 170 220 2700 0.5 1.0 0.03 T , KT , KT M , e m u/ g M , e m u/ g YSr Co O3 4 10.5+δ Fig. 7. Temperature dependences of the magnetization for Sr3.2Y0.8Co4O10.5+δ (1), Sr3YCo4O10.5+δ (2), and Sr2.6Y1.4Co4O10.5+δ (3) samples (H = 1 T). 0 50 100 150 200 250 300 0 2 4 6 H = 1 T 1 2 3 , KT M , e m u/ g I.O. Troyanchuk, M.V. Bushinsky, D.V. Karpinsky, and V.A. Sirenko 840 Low Temperature Physics/Fizika Nizkikh Temperatur, 2012, v. 38, No. 7 The ferromagnetic component is associated with noncol- linear magnetic structure. 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