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Register a new userFerroelectricity of structural origin in spin-chain compounds Ca$_3$Co$_{2-x}$Mn$_x$O$_6$
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We report a systematic study of the structure, electric and magnetic properties of Ca$_3$Co$_{2-x}$Mn$_x$O$_6$ single crystals with $x =$ 0.72 and 0.26. The DC and AC magnetic susceptibilities display anomalies with characteristic of the spin freezing. The crystals show ferroelectric transition at 40 K and 35 K ($T_{FE}$) for $x =$ 0.72 and 0.26, respectively, with a large value of 1400 $mu$C/m$^2$ at 8 K for electric polarization ($P_c$) along the spin-chain ($c$-axis) direction. Interestingly, the electric polarization perpendicular to the chain direction ($P_{ab}$) can also be detected and has value of 450 and 500 $mu$C/m$^2$ at 8 K for the $x =$ 0.72 and 0.26 samples, respectively. The specific heat and magnetic susceptibility show no anomaly around $T_{FE}$, which means that the electric polarization of these samples has no direct relationship with the magnetism. The X-ray diffraction and the Raman spectroscopy indicate that these samples may undergo Jahn-Teller distortions that could be the reason of electric polarization.
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The origin of both the Ising chain magnetism and ferroelectricity in Ca$_3$CoMnO$_6$ is studied by $ab$ $initio$ electronic structure calculations and x-ray absorption spectroscopy. We find that Ca$_3$CoMnO$_6$ has the alternate trigonal prismatic Co$^{2+}$ and octahedral Mn$^{4+}$ sites in the spin chain. Both the Co$^{2+}$ and Mn$^{4+}$ are in the high spin state. In addition, the Co$^{2+}$ has a huge orbital moment of 1.7 $mu_B$ which is responsible for the significant Ising magnetism. The centrosymmetric crystal structure known so far is calculated to be unstable with respect to exchange striction in the experimentally observed $uparrowuparrowdownarrowdownarrow$ antiferromagnetic structure for the Ising chain. The calculated inequivalence of the Co-Mn distances accounts for the ferroelectricity.
Layered perovskites $A_3M_2$O$_7$ are known to exhibit the so-called hybrid improper ferroelectricity. Despite experimentally confirmed cases (e.g. nonmagnetic $M$=Ti and Sn), the ferroelectricity in magnetic Ca$_3$Mn$_2$O$_7$ remains a puzzle. Here, the structural, ferroelectric, magnetoelectric, and optical properties of Ca$_3$Mn$_2$O$_7$ are systematically investigated. Switchable polarization is directly measured, demonstrating its ferroelectricity. In addition, magnetoelectric response is also evidenced, implying the coupling between magnetism and ferroelectricity. Furthermore, strong visible light absorption is observed, which can be understood from its electronic structure. Its direct and appropriate band gap, as well as wide conducting bands, makes Ca$_3$Mn$_2$O$_7$ a potential candidate for ferroelectric photoelectric applications.
We have studied the effect of Al doping on the structural, magnetic and electrical properties of La$_{1-x}$Ba$_x$Mn$_{1-x}$Al$_x$O$_3$ ($0leq x leq 0.25$) manganite, annealed in two 750$^oC$ and 1350$^oC$ temperatures. The XRD analysis shows that the structures in all samples have single phase rhombohedral structure with R$bar{3}$c space group. The unit cell volume almost decrease with increasing the Al doping in all samples. The grain growth with increasing annealing temperature and Al doping also have been studied. We observed that, T$_c$ temperature decreases when the Al ion substitute in Mn ion site. The magnetic study of the samples via magnetic susceptibility results in Griffiths and spin-glass phase for samples doped with aluminium. Along the resistivity measurement results, the $T_{MIT}$ (metal-insulator) transition temperatures decrease and the system become an insulator. The insulator-metal transition occurs for L0 sample in near 165K, while this transition is weak for H0 sample due to oxygen non-stoichiometry.Using three models viz. 1. Adiabatic small polaron hoping, 2.Variable range hopping, and 3. Percolation model, the resistance have been studied.
The valence and spin state evolution of Mn and Co on TbMn$_{rm 1-x}$Co$_{rm x}$O$_3$ series is precisely determined by means of soft and hard x-ray absorption spectroscopy (XAS) and K$beta$ x-ray emission spectroscopy (XES). Our results show the change from Mn$^{3+}$ to Mn$^{4+}$ both high-spin (HS) together with the evolution from Co$^{2+}$ HS to Co$^{3+}$ low-spin (LS) with increasing $rm x$. In addition, high energy resolution XAS spectra on the K pre-edge region are interpreted in terms of the strong charge transfer and hybridization effects along the series. These results correlate well with the spin values of Mn and Co atoms obtained from the K$beta$ XES data. From this study, we determine that Co enters into the transition metal sublattice of TbMnO$_3$ as a divalent ion in HS state, destabilizing the Mn long range magnetic order since very low doping compositions (${rm x} le 0.1$). Samples in the intermediate composition range ($0.4 le {rm x} le 0.6$) adopt the crystal structure of a double perovskite with long range ferromagnetic ordering which is due to Mn$^{4+}$-O-Co$^{2+}$ superexchange interactions with both cations in HS configuration. Ferromagnetism vanishes for ${rm x} ge 0.7$ due to the structural disorder that collapses the double perovskite structure. The spectroscopic techniques reveal the occurrence of Mn$^{4+}$ HS and a fluctuating valence state Co$^{2+}$ HS/Co$^{3+}$ LS in this composition range. Disorder and competitive interactions lead to a magnetic glassy behaviour in these samples.
A neutron scattering study of nonsuperconducting La$_{2-x}$Sr$_x$CaCu$_2$O$_6$ (x=0 and 0.2), a bilayer copper oxide without CuO chains, has revealed an unexpected tetragonal-to-orthorhombic transition with a doping dependent transition temperature. The predominant structural modification below the transition is an in-plane shift of the apical oxygen. In the doped sample, the orthorhombic superstructure is strongly disordered, and a glassy state involving both magnetic and structural degrees of freedom develops at low temperature. The spin correlations are commensurate.
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