The influence of the A-site ionic radii (<rA>) on the magnetic structure has been investigated in La0.5Ca0.5-xSrxMnO3 compounds (0 .GE. x .LE. 0.5) using neutron diffraction, magnetization, and resistivity techniques. All compounds in the composition range x .LE. 0.3 crystallize in the orthorhombic structure (Space Group Pnma). No further structural transition is observed as temperature is lowered below 300K. The compound x = 0.4, is a mixture of two orthorhombic phases crystallizing in Pnma and Fmmm space group. The x = 0.5 compound has a tetragonal structure in the space group, I4/mcm. The charge ordered (CO) state with CE-type antiferromagnetic order remains stable for x .LE. 0.3. Above x = 0.3, the CE-type antiferromagnetic state is suppressed. In x = 0.4 compound, A-type antiferromagnetic ordering is found at temperatures below 200K. Orbital ordering accompanying the spin ordering is found in all the samples with x .LE. 0.4. The system becomes ferromagnetic at x = 0.5 and no signature of orbital ordering is observed. As a function of <rA>, the charge ordered state is stable up to <rA> ~ 1.24A, and is suppressed thereafter. The magnetic structure undergoes a transformation from CE-type antiferromagnetic state to a ferromagnetic state with an intermediate A-type antiferromagnetic state.
The effect of quenched disorder on the multiphase competition has been investigated by examining the pressure phase diagram of half doped manganite Ln0.5B0.5MnO3 (Ln = Sm and Nd) with A-site disorders. Sm0.5Ba0.5MnO3, a spin glass insulator at ambient pressure, switches to a ferromagnetic metal with increasing pressure, followed by a rapid increase of the ferromagnetic transition temperature Tc. The rapid increase of Tc was confirmed also for Nd0.5Ba0.5MnO3. These observations indicate that the unusual suppression of the multicritical phase boundary in the A-site disordered system, previously …
Correlation between orbital structure and magnetic ordering in bilayered manganites is examined. A level separation between the $3d_{3z^2-r^2}$ and $3d_{x^2-y^2}$ orbitals in a Mn ion is calculated in the ionic model for a large number of the compounds. It is found that the relative stability of the orbitals dominates the magnetic transition temperatures as well as the magnetic structures. A mechanism of the correlation between orbital and magnetism is investigated based on the theoretical model with the two $e_g$ orbitals under strong electron correlation.
The field induced switching of conductance in the charge ordered half-doped manganites is controlled by the combination of metastability, an inhomogeneous high field state, and cation disorder. We study this non-equilibrium problem via real space Monte Carlo on a disordered strong coupling model appropriate to the manganites. We reproduce the variation of the switching fields with the mean ionic radius r_A and cation disorder σ_A, and demonstrate how the experimental features arise from the proximity of several phases in the Landau free energy landscape. Our prediction for the field melted sta…
Transition-metal perovskite oxides exhibit a wide range of extraordinary but imperfectly understood phenomena. Charge, spin, orbital, and lattice degrees of freedom all undergo order-disorder transitions in regimes not far from where the best-known of these phenomena, namely high-temperature superconductivity of the copper oxides, and the 'colossal' magnetoresistance of the manganese oxides, occur. Mostly diffraction techniques, sensitive either to the spin or the ionic core, have been used to measure the order. Unfortunately, because they are only weakly sensitive to valence electrons and yie…
Through analysis of variable temperature neutron powder diffraction data, we present solutions for the magnetic structures of SrMn$_7$O$_{12}$, CdMn$_7$O$_{12}$, and PbMn$_7$O$_{12}$ in all long-range ordered phases. The three compounds were found to have magnetic structures analogous to that reported for CaMn$_7$O$_{12}$. They all feature a higher temperature lock-in phase with \emph{commensurate} magneto-orbital coupling, and a delocked, multi-\textbf{k} magnetic ground state where \emph{incommensurate} magneto-orbital coupling gives rise to a constant-moment magnetic helix with modulated sp…
A model of chemical bonding between ions in manganites involving covalent one-electron $σ$ bonding is suggested. The covalent one-electron $σ$ bonding gives rise to a strongly correlated state of electrons resulting from the exchange interaction between electrons when they are simultaneously at cation and anion orbitals. The manifestation of the correlatred state is the spin and spatial ordering of the electrons resulting in the formation of a spin- ordered electron lattice. The conductivity of manganites in this model is the consequence of displacement of the electron lattice (or its part) fr…
Versatile features of impurity doping effects on perovskite manganites, $R_{0.6}$Sr$_{0.4}$MnO$_{3}$, have been investigated with varying the doing species as well as the $R$-dependent one-electron bandwidth. In ferromagnetic-metallic manganites ($R$=La, Nd, and Sm), a few percent of Fe substitution dramatically decreases the ferromagnetic transition temperature, leading to a spin glass insulating state with short-range charge-orbital correlation. For each $R$ species, the phase diagram as a function of Fe concentration is closely similar to that for $R_{0.6}$Sr$_{0.4}$MnO$_{3}$ obtained by de…
Detailed investigations of structural, magnetic and electronic transport properties of hole-doped high-entropy rare-earth manganites are presented. The high-entropy samples (LaNdPrSmEu)$_{1-x}$Sr$_x$MnO$_3$ (0$\leq$\textit{x}$\leq$0.5), synthesized using the solid-state technique, show a change in the crystal structure from \textit{Pbnm} to \textit{R-3c} with increasing Sr substitution, attributed to the change in the tolerance factor. Prominent ferromagnetic ordering is observed in the sample with a rhombohedral structure (\textit{x}$\geq$0.3), originating from the dominant double exchange me…
The discovery of novel structural and physical properties in the $A$-site ordered manganite $R$BaMn$_{2}$O$_{6}$ ($R$ = Y and rare earth elements) has demanded new comprehension about perovskite manganese oxides. In the present study, the $A$-site disordered form, $R_{0.5}$Ba$_{0.5}$MnO$_{3}$, has been investigated and compared with both $R$BaMn$_{2}$O$_{6}$ and $R_{0.5}A_{0.5}$MnO$_{3}$ ($A$: Sr, Ca) in the structures and electromagnetic properties. $R_{0.5}$Ba$_{0.5}$MnO$_{3}$ has a primitive cubic perovskite cell in the structure and magnetic glassy states are dominant as its ground state, …
The effect of Pr-doping on structural, magnetic and transport properties in electron-doped manganites La0.9-xPrxTe0.1MnO3 with fixed carrier concentration are investigated. The room temperature structural transition from rhombohedral (R3C) to orthorhombic (Pbnm) symmetry is found in the samples with by the Rietveld refinement of x-ray powder diffraction patterns. The Curie temperature of samples decreases and the transition becomes broader with increasing Pr-doping level. For the samples with, there exist insulator-metal (I-M) transition. And the low-temperature I-M transition is observed at a…
We use ab initio electronic structure calculations within the generalized gradient approximation (GGA+U) to density functional theory (DFT) to determine the microscopic exchange interactions in the series of orthorhombic rare-earth manganites, o-$R$MnO$_3$. Our motivation is to construct a model Hamiltonian (excluding effects due to spin-orbit coupling), which can provide an accurate description of the magnetism in these materials. First, we consider TbMnO$_3$, which exhibits a spiral magnetic order at low temperatures. We map the exchange couplings in this compound onto a Heisenberg Hamiltoni…
The effect of Fe substitution on Mn sites in the colossal magnetoresistive compounds La0.65Ca0.35Mn1-xFexO3 with 0.01<x<0.1 have been studied. A careful study in the magnetic properties has been carried out by the measurement of ac susceptibility. The temperature range of CMR is greatly broadened with the addition of Fe. Substitution of Fe induces a gradual transition from a metallic ferromagnetic with a high Curie temperature (Tc=270 K) to a ferromagnetic insulator with low Tc=79 K. Increased spin disorder and decrease of Tc with increasing Fe content are evident. The variations in the critic…
We have established detailed magnetoelectric phase diagrams of (Eu$_{0.595}$Y$_{0.405}$)$_{1-x}$Tb$_x$MnO$_3$ ($0 \le x \le 1$) and (Eu,Y)$_{1-x}$Gd$_x$MnO$_3$ ($0 \le x \le 0.69$), whose average ionic radii of $R$-site ($R$: rare earth) cations are equal to that of Tb$^{3+}$, in order to reveal the effect of rare earth 4$f$ magnetic moments on the magnetoelectric properties. In spite of the same $R$-site ionic radii, the magnetoelectric properties of the two systems are remarkably different from each other. A small amount of Tb substitution on $R$ sites ($x \sim 0.2$) totally destroys ferroel…
We present first principles LDA+U calculations of electronic structure and magnetic state for LaCoO3 and HoCoO3. Low Spin to Intermediate Spin state transition was found in our calculations using experimental crystallographic data for both materials with a much higher transition temperature for HoCoO3, which agrees well with the experimental estimations. Low Spin state t6e0 (non-magnetic) to Intermediate Spin state t5e1 (magnetic) transition of Co(3+) ions happens due to the competition between crystal field t_2g-e_g splitting and effective exchange interaction between 3$d$ spin-orbitals. We s…
The emergence of superlattice periodicities at metal to insulator transitions in hole doped perovskite oxides responds to a rearrangement of the local atomic structure, and electron and spin density distribution. Originally, the ionic model based on a checkerboard- type atomic distribution served to describe the low temperature charge and orbital ordered (COO) phases arising in half- doped manganites. In the last years, the exploitation of resonant x- ray scattering (RXS) capabilities has shown the need to revisit these concepts and improve the picture. Yet, we have realised that COO is a more…
Mn site is substituted with closed shell ions (Al, Ga. Ti, Zr and a certain combination of Zr and Al) and also with Fe and Ru ions carrying the magnetic moment (S=5/2 and 2 respectively) at a fixed concentration of 5 at. %. Substitution did not change either the crystal symmetry or the oxygen stiochiometry. All substituents were found to suppress both the metal-insulator and ferromagnetic transition temperatures (TP(r) and TC respectively) to varied extents. Two main contributions identified for the suppression are the lattice disorder arising due to difference in the ionic radii (rMn3+-rM) be…
We report the effect of Al substitution on the Mn site of the bilayered half doped manganite La{_1}Sr{_2}Mn{_2}O{_7}. This substitution dilutes the magnetically active Mn-O-Mn network without introducing an appreciable distortion in the lattice and ionic considerations leads to a predominant reduction of Mn{^{4+}} with increasing Al. The rate of fall of the long range antiferromagnetic transition temperature as a function of substitution is seen to match well with established quasi 2D Heisenberg systems indicating that the nature of magnetic interactions in this quasi 2-D system is of the shor…
We report structural, magnetic and dielectric properties of layered perovskite materials LnBaCuFeO5 (Ln = La and Lu). LaBaCuFeO5 shows magnetic cluster glass behavior below 60 K owing to the competing ferromagnetic and antiferromagnetic exchange interactions. Glassy dynamics of electric dipoles has also been observed in the vicinity of the magnetic glass transition temperature. The presence of significant coupling between spin and polar degrees of freedom results in the multiglass feature in LaBaCuFeO5. The LuBaCuFeO5 compound undergoes YBaCuFeO5 like commensurate to incommensurate antiferroma…
We have investigated the effect of site dilution with substitution of nonmagnetic element in SrRu$_{1-x}$Ti$_x$O$_3$ ($x$ $\leq$ 0.7). The nature of ferromagnetic state in SrRuO$_3$ is believed to be of itinerant type with transition temperature $T_c$ $\sim$ 162 K. Crystallographically, SrRuO$_3$ has a distorted orthorhombic structure. Substitution of Ti$^{+4}$ (3$d^0$) for Ru$^{+4}$ (4$d^4$), however, does not introduce significant structural modification due to their matching ionic radii. This substitution, on the other hand, is expected to tune the electronic correlation effect and the $d$ …
Here, we report an evolution of structural, magnetic and transport behavior in doped SrRu$_{1-x}$Ga$_x$O$_3$ ($x$ $\le$ 0.2). The nonmagnetic dopant Ga$^{3+}$ (3$d^{10}$) not only acts for magnetic site dilution in SrRuO$_3$ but also it modifies the Ru charge state and electronic density. Our studies show that Ga$^{3+}$ substitution does not affect the original orthorhombic-\textit{Pbnm} structure of SrRuO$_3$ which is due to its matching ionic radii with Ru$^{4+}$. However, Ga$^{3+}$ has a substantial effect on the magnetic behavior of SrRuO$_3$ where it decreases both magnetic moment as well…
The delicate balance between spin-orbit coupling, Coulomb repulsion and crystalline electric field interactions observed in Ir-based oxides is usually manifested as exotic magnetic behavior. Here we investigate the evolution of the exchange coupling between Co and Ir for partial La substitution by Ca in La$_{2}$CoIrO$_6$. A great advantage of the use of Ca$^{2+}$ as replacement for La$^{3+}$ is the similarity of its ionic radii. Thus, the observed magnetic changes can more easily be associated to electronic variations. A thorough investigation of the structural, electronic and magnetic propert…
