High entropy BaFe12-x(Ti/Mn/Ga/In)xO19 (x = 1–7) oxides: Correlation of the composition, entropy state, magnetic characteristics, and terahertz properties

Abstract

The BaFe12-x (Ti/Mn/Ga/In)xO19 (x = 1–7) high-entropy oxides (HEOs) were obtained by solid-phase synthesis. The correlation of the chemical composition (the level of the Fe replacement), structural parameters, magnetic characteristics, and terahertz (THz) properties was investigated. All studied samples were single-phase (SG: P63/mmc). Lattice parameters showed a monotonic increasing trend with an increase of (x). The key role in increasing the lattice parameters of HEOs may belong to the influence of In3+ ions, which are much larger in size than Fe3+ ions. As one of the possible reason for explanation of the lattice parameters behavior we hypothesized that partial charge transformation of the Mn3+ state to the Mn2+ state takes place in order to maintain electrical neutrality. Other cations (Ti/Ga/In) have stable oxidation state. The anisotropic nature of the increase in lattice parameters was demonstrated. No strong correlation between chemical composition and microstructural parameters of the investigated HEOs was observed. The magnetic characteristics of the BaFe12-x (Ti/Mn/Ga/In)xO19 (x = 1–7) HEOs were investigated at broad intervals of magnetic fields and temperatures. The behavior of the magnetic characteristics was shown to be the result of the magnetic structure frustration. In addition, terahertz electrodynamic properties were studied by measuring spectra of complex dielectric permittivity at frequencies 0.2–1.2 THz in the temperature interval 20–300 K. The spectra indicate the presence of a higher-frequency infrared phonon resonance, whose damping decreases with cooling, as well as an excitation below 0.2 THz that freezes out at low temperatures, the origin of which is associated with the polycrystalline nature of the materials.