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Register a new userA rock-salt type Li-based oxide, Li3Ni2RuO6, exhibiting a chaotic ferrimagnetism with cluster spin-glass dynamics and thermally frozen charge carriers
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E. V. Sampathkumaran Professor
Publication date
2016
fields
Physics
and research's language is
English
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The area of research to discover new Li containing materials and to understand their physical properties has been of constant interest due to applications potential for rechargeable batteries. Here, we present the results of magnetic investigations on a Li compound, Li3Ni2RuO6, which was believed to be a ferrimagnet below 80K. While our neutron diffraction (ND) and isothermal magnetization (M) data support ferrimagnetism, more detailed magnetic studies establish that this ferrimagnetic phase exhibits some features similar to spin-glasses. In addition, we find another broad magnetic anomaly around 40-55 K in magnetic susceptibility, attributable to cluster spin-glass phenomenon. Gradual dominance of cluster spin-glass dynamics with a decrease of temperature (T) and the apparent spread in freezing temperature suggest that the ferrimagnetism of this compound is a chaotic one. The absence of a unique freezing temperature for a crystalline material is interesting. In addition, pyroelectric current data reveals a feature in the range 40-50 K, attributable to thermally stimulated depolarization current. We hope this finding motivates future work to explore whether there is any intriguing correlation of such a feature with spin-glass dynamics. We attribute these magnetic and electric dipole anomalies to the crystallographic disorder intrinsic to this compound.
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Li5OsO6 and Li5ReO6 polycrystalline samples were synthesized by conventional solid state methods. Employing powder neutron diffraction data, the crystal structure of Li5OsO6 was re-investigated. Li5OsO6 crystallizes in C2/m space group in an ordered NaCl structure type where a = 5.0472(1) A, b = 8.7827(2) A, c = 5.0079(1) A, Beta = 109.777(2) degree and V = 208.90(1).A^3 Magnetic susceptibility and heat capacity data indicate an AFM long range order below 40K although there is evidence for low dimensional short range order above 80K. As well, the frustration index, f = |theta|/TN ~1, in contrast to the isostructural and isoelectronic compound, Li4MgReO6, which is a spin glass below 12K and has f ~ 14. An attempt was made to rationalize these differences using spin dimer analysis. The key results are that the spin exchange interactions in the Re-based compound are stronger and are consistent with a frustrated triangular lattice model while a low dimensional short range order model is better for Li5OsO6. The main reason for this is a strong Jahn-Teller distortion in the OsO6 octahedron material which constrains the unpaired electron to occupy the dxy orbital.
We report the results of neutron diffraction, ac and dc magnetization, heat-capacity, complex permittivity, and pyrocurrent measurements on an oxide, Li3NiRuO5, hitherto not paid much attention in the literature, except for a previous report on its promising electrochemical performance. We emphasize on the following findings: (i) Observation of re-entrant spin-glass behavior; that is, this oxide undergoes ferrilmagnetic ordering below 8- K, entering spin-glass regime around 12 K. (ii) There is no prominent feature in the complex dielectric permittivity (in particular, at the magnetic transitions) in the absence of external magnetic field, indicative of the absence of ferroelectricity. However, there is a distinct evidence for magneto-dielectric (MDE) coupling. The sign of MDE coupling also changes as the sample is cooled from ferrimagnetic state to spin-glass regime. (iii) There are pyroelectric anomalies in the vicinity of 30-70 K, presumably from thermally stimulated depolarization current.
The results of dc and ac magnetization, heat-capacity, 57Fe Moessbauer spectroscopy, dielectric, pyroelectric current and isothermal magneto-capacitance measurements on a recently reported lithium-based oxide, Li3FeRuO6, related to LiCoO2-type rhombohedral structure (space group, R-3m) are presented. The results reveal that the compound undergoes spin-glass freezing below 15 K. There is a peak around 34 K in pyroelectric data, which can not be attributed to ferroelectricity, but to the phenomenon of thermally stimulated depolarization current. As revealed by magnetocapacitance data above and below magnetic ordering temperature, magnetic and electric dipoles appear to be coupled, thereby offering evidence for magnetodielectric coupling.
An oxygen hyperstoichiometric ferrite CaBaFe4O7+delta (delta approx 0.14) has been synthesized using soft reduction of CaBaFe4O8. Like the oxygen stoichiometric ferrimagnet CaBaFe4O7, this oxide also keeps the hexagonal symmetry (space group: P63mc), and exhibits the same high Curie temperature of 270 K. However, the introduction of extra oxygen into the system weakens the ferrimagnetic interaction significantly at the cost of increased magnetic frustration at low temperature. Moreover, this canonical spin glass (Tg ~ 166 K) exhibits an intriguing cross-over from de Almeida-Thouless type to Gabay-Toulouse type critical line in the field temperature plane above a certain field strength, which can be identified as the anisotropy field. Domain wall pinning is also observed below 110 K. These results are interpreted on the basis of cationic disordering on the iron sites.
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