We present a detailed dielectric study of the relaxation effects that occur in several perovskite rare-earth manganites, including the multiferroics TbMnO3 and DyMnO3. We demonstrate that the strong magnetocapacitive effects, observed for electrical fields E||c, are nearly completely governed by magnetic-state induced changes of the relaxation parameters. The multiferroic materials, which undergo a transition into a spiral magnetic state, show qualitatively different relaxation behavior than those compounds transferring into an A-type antiferromagnetic state. We ascribe the relaxations in both cases to the off-center motion of the manganese ions, which in the multiferroic systems also leads to the ferroelectric ordering.
Many multiferroic materials, with various chemical compositions and crystal structures, have been discovered in the past years. Among these multiferroics, some perovskite manganites with ferroelectricity driven by magnetic orders are of particular interest. In these multiferroic perovskite manganites, not only their multiferroic properties are quite prominent, but also the involved physical mechanisms are very plenty and representative. In this Brief Review, we will introduce some recent theoretical and experimental progress on multiferroic manganites.
We present a detailed study of a model for strain-induced metal-insulator phase coexistence in perovskite manganites. Both nanoscale and mesoscale inhomogeneities are self-consistently described using atomic scale modes and their associated constraint equations. We also examine the stability of domain configurations against uniform and nonuniform modifications of domain walls. Our results show that the long range interactions between strain fields and the complex energy landscape with multiple metastable states play essential roles in stabilizing metal-insulator phase coexistence, as observed …
Roles of orbital degree of freedom of Mn ions in phase transition as a function of temperature and hole concentration in perovskite manganites are studied. It is shown that the orbital order-disorder transition is of the first order in the wide region of hole concentration and the N$\rm \acute{e}$el temperature for the anisotropic spin ordering, such as the layer-type antiferromagnetic one, is lower than the orbital ordering temperature due to the anisotropy in the orbital space. The calculated results of the temperature dependence of the spin and orbital order parameters explain a variety of …
We discovered an unprecedented magnitude of the 1/f noise near the Curie temperature Tc in low-Tc manganites. The scaling behavior of the 1/f noise and the resistance provides strong evidence of the percolation nature of the ferromagnetic transition in the polycrystalline samples. The step-like changes of the resistance with temperature, observed for single crystals, suggest that the size of the ferromagnetic domains depends on the size of crystallites.
The double exchange model describing the coupling between conduction electrons and localized magnetic moments is relevant for a large family of physical systems including manganites. Here we reveal that the one dimensional double exchange model with an incommensurate magnetic elliptical spiral is a topological insulator with a Chern number $2\mathbb{Z}$ in the two dimensional space with one physical dimension and one ancillary dimension spanned by the Goldstone mode of the spiral. Moreover, the electronic states can be localized for a strong local exchange coupling. The topological protected e…
This paper reports the observations of long-time relaxation, aging, and temperature memory behaviors of resistance and magnetization in the ferromagnetic state of a polycrystalline La0.7Ca0.3Mn0.925Ti0.075O3 compound. The observed glassy dynamics of the electrical transport appears to be magnetically originated and has a very close association with the magnetic glassiness of the sample. Phase separation and strong correlation between magnetic interactions and electronic conduction play the essential roles in producing such a resistive glassiness. We explain the observed effects in terms of a c…
We report a detailed study of step-like metamagnetic transitions in the magnetization and resistivity of polycrystalline Pr0.5Ca0.5Mn0.95Co0.05O3. The steps have a sudden onset below a critical temperature, are extremely sharp (width < 0.2 mT), and occur at critical fields which are linearly dependent on the absolute value of the cooling field in which the sample is prepared. Similar transitions are also observed at low temperature in non-Co doped manganites, including single crystal samples. These data show that the steps are an intrinsic property, qualitatively different from either previous…
In this work the charge transport properties of charge ordered (CO) La1-xCaxMnO3 (LCMO) (x= 0.55, 0.67) epitaxial thin films and polycrystals are discussed following the recent controversy of localised electron states vs. weakly or de- localised charge density wave (CDW) states in CO manganites. The transport properties were investigated by current vs. voltage, direct current resistivity vs. temperature, local activation energy vs. temperature, magnetoresistance and admittance spectroscopy measurements, which all indicated a localised electronic structure in the single CO phase. Delocalised ch…
Temperature dependent optical conductivity spectra of a La0.7Ca0.3MnO3 (LCMO) sample were measured. In the metallic regime at very low temperatures, they clearly showed two types of absorption features, i.e., a sharp Drude peak and a broad mid-infrared absorption band, which could be explained as coherent and incoherent bands of a large lattice polaron. This elementary excitation in LCMO was found to be in a strong coupling regime and to have interactions with the spin degree of freedom.
We report an interesting reentrant metallic resistivity pattern beyond a characteristic temperature T* which is higher than other such characteristic transition temperatures like T(c)(Curie point), T(N) (Neel point), T(CO) (charge order onset point) or T(OO) (orbital order onset point) in a range of rare-erath perovskite manganites (RE(1-x)A(x)MnO(3); RE = La, Nd, Y; A = Sr, Ca; x = 0.0-0.5). Such a behavior is normally observed in doped manganites with doping level (x) higher than the critical doping level x(c) (= 0.17-0.22) required for the metallic ground state to emerge and hence in a syst…
Magnetoelectric phase diagrams of the perovskite manganites, Eu1-xYxMnO3 and Gd1-xTbxMnO3, are theoretically studied. We first construct a microscopic model, and then analyze the model using the Monte-Carlo method. We reproduce the diagrams, which contain two different multiferroic states, i.e., the ab-plane spin cycloid with electric polarization P//a and the bc-plane spin cycloid with P//c. We reveal that their competition originates from a conflict between the single-ion anisotropy and the Dzyaloshinsky-Moriya interaction, which is controlled by the second-neighbor spin exchanges enhanced b…
We present a theoretical study on the relation between the size of the rare earth ions, often known as chemical pressure, and the stability of the coherent Jahn-Teller distortions in undoped perovskite manganites. Using a Keating model expressed in terms of atomic scale symmetry modes, we show that there exists a coupling between the uniform shear distortion and the staggered buckling distortion within the Jahn-Teller energy term. It is found that this coupling provides a mechanism by which the coherent Jahn-Teller distortion is more stabilized by smaller rare earth ions. We analyze the appear…
Variation of magnetocaloric (MC) effects has been systematically investigated for colossal magnetoresistive (CMR) manganites R0.6Sr0.4MnO3 (R=La-Gd). As the one-electron bandwidth is reduced, the temperature profile of MC effect, i.e., field-induced entropy change, exhibits a steeper drop below the ferromagnetic transition temperature due to its first-order nature promoted by a competing charge-orbital ordering instability. For these small-bandwidth systems adjacent to the metal-insulator phase boundary, a rectangular-shaped profile for the entropy change emerges with an anomalously wide tempe…
We have performed both theoretical and experimental study of optical response of parent perovskite manganites RMnO_3 with a main goal to elucidate nature of clearly visible optical features. Starting with a simple cluster model approach we addressed the both one-center (p-d) and two-center (d-d) charge transfer (CT) transitions, their polarization properties, the role played by structural parameters, orbital mixing, and spin degree of freedom. Optical complex dielectric function of single crystalline samples of RMnO_3 (R=La, Pr, Nd, Sm, Eu) was measured by ellipsometric technique at room tempe…
The effect of cobalt and nickel substitutions for manganese on the physical properties of the perovskite manganite La1.2Bi0.8Mn2-x(Ni/Co)xO6+d, with x = 0.0-0.8, has been investigated. It is observed that the ferromagnetism is enhanced, TC being increased from 103 K for the parent compound (x = 0.0) to 178 K for Ni-phase, and to 181 K for the Co-phase (x = 0.8). Moreover, the systems remain insulating and depict relatively large values of magnetoresistance effect at low temperatures (up to 67 % at 90K and 70 kOe, for x = 0.0 phase). These phenomena are interpreted by means of electronic phase …
A unified theory is developed to explain various types of electronic collective behaviors in doped manganites R$_{1-x}$X$_x$MnO$_3$ (R = La, Pr,Nd etc. and X = Ca, Sr, Ba etc.). Starting from a realistic electronic model, we derive an effective Hamiltonianis by ultilizing the projection perturbation techniques and develop a spin-charge-orbital coherent state theory, in which the Jahn-Teller effect and the orbital degeneracy of e$_g$ electrons in Mn ions are taken into account. Physically, the experimentally observed charge ordering state and electronic phase separation are two macroscopic quan…
We compute the zero temperature phase diagram and the Hall response of the doped perovskite manganites within the model of double exchange and Jahn-Teller coupling, employing the large dimensionality approximation proposed by Millis et al. We find that in this scenario a ``hole - like'' $R_H$ for the hole doped manganites, as observed at low temperature by Matl et al., can be obtained only when lattice distortions persist in the metallic state at zero temperature. The calculated temperature dependence of $R_H$ seems to be consistent with the measured ``normal'' Hall coefficient in thin films.
We present the discovery and refinement by neutron powder diffraction of a new magnetic phase in the Na1-xCaxMn7O12 quadruple perovskite phase diagram, which is the incommensurate analogue of the well-known pseudo-CE phase of the simple perovskite manganites. We demonstrate that incommensurate magnetic order arises in quadruple perovskites due to the exchange interactions between A and B sites. Furthermore, by constructing a simple mean field Heisenberg exchange model that generically describes both simple and quadruple perovskite systems, we show that this new magnetic phase unifies a picture…
Complete magnetoelectric (ME) phase diagrams of orthorhombic $R$MnO$_{3}$ with and without magnetic moments on the $R$ ions have been established. Three kinds of multiferroic ground states, the $ab$-cycloidal, the $bc$-cycloidal, and the collinear $E$-type phases, have been identified by the distinct ME responses. The electric polarization of the $E$-type phase dominated by the symmetric spin exchange ($bm{S}_{i} cdot bm{S}_{j}$) is more than 10 times as large as that of the $bc$-cycloidal phase dominated by the antisymmetric one ($bm{S}_{i} times bm{S}_{j}$), and the ME response is enhanced n…
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, …
Measurements of the low-frequency (f<=100 kHz) permittivity and conductivity at T<= 150 K are reported for La(1-x)Ca(x)MnO(3) (0<=x<=1) and Ca(1-y)Sr(y)MnO(3) (0<=y<=0.75) having antiferromagnetic, insulating ground states covering a broad range of Mn valencies from Mn(3+) to Mn(4+). Static dielectric constants are determined from the low-T limiting behavior. With increasing T, relaxation peaks associated with charge-carrier hopping are observed in the real part of the permittivities and analyzed to determine dopant binding energies. The data are consistent with a simple model of hydrogenic im…
Optical conductivity spectra of La_{0.7-y}Pr_{y}Ca_{0.3}MnO_3 were systematically investigated. For metallic samples, the spectral weight below 0.5 eV, whose magnitude can be represented by the effective carrier number N_{eff}(0.5 eV), increases as temperature becomes lower. Regardless of the Pr doping, all the measured values of N_{eff}(0.5 eV)/T_C fall into one scaling curve. This scaling behavior could be explained by the theoretical model by Roeder et al. [Phys. Rev. Lett. 76, 1356 (1996)], which includes spin double exchange and Jahn-Teller lattice coupling to holes. With the Pr doping, f…
Orthorhombically distorted perovskite manganites, RMnO3 with R being a trivalent rare-earth ion, exhibit a variety of magnetic and electric phases including multiferroic (i.e. concurrently magnetic and ferroelectric) phases and fascinating magnetoelectric phenomena. We theoretically study the phase diagram of RMnO3 by constructing a microscopic spin model, which includes not only the superexchange interaction but also the single-ion anisotropy (SIA) and the Dzyaloshinsky-Moriya interaction (DMI). Analysis of this model using the Monte-Carlo method reproduces the experimental phase diagrams as …
Structural study of orbital-ordered manganite thin films has been conducted using synchrotron radiation, and a ground state electronic phase diagram is made. The lattice parameters of four manganite thin films, Nd0.5Sr0.5MnO3 (NSMO) or Pr0.5Sr0.5MnO3 (PSMO) on (011) surfaces of SrTiO3 (STO) or [(LaAlO3){0.3}(SrAl0.5Ta0.5O3){0.7}] (LSAT), were measured as a function of temperature. The result shows, as expected based on previous knowledge of bulk materials, that the films' resistivity is closely related to their structures. Observed superlattice reflections indicate that NSMO thin films have an…
In order to reveal many-body interactions in the three-dimensional (3D) perovskite manganite, we have performed an $in$ $situ$ angle-resolved photoemission spectroscopy (ARPES) on La$_{0.6}$Sr$_{0.4}$MnO$_3$ (LSMO) and investigated the behaviors of quasiparticles. We observe quasiparticle peaks around the Fermi momentum, both in the electron and the hole bands, and clear kinks throughout the hole Fermi surface in the ARPES band dispersion. The isotropic behavior sharply contrasts to the strong anisotropic quasiparticle excitation observed in layered manganites. These results suggest that polar…
We have studied the sub-picosecond quasiparticle dynamics in the perovskite manganite La0.7Ca0.3MnO3 and the layered manganite La1.4Sr1.6Mn2O7 using ultrafast optical spectroscopy. We found that for T > TC, initial relaxation proceeds on the time scale of several hundred femtoseconds and corresponds to the redressing of a photoexcited electron to its polaronic ground state. The temperature and dimensionality dependence of this polaron redressing time provides insight into the relationship between polaronic motion and spin dynamics on a sub-picosecond time scale. We also observe a crossover to …
Femtosecond reflection spectroscopy was performed on a perovskite-type manganite, Gd0.55Sr0.45MnO3, with the short-range charge and orbital order (CO/OO). Immediately after the photoirradiation, a large increase of the reflectivity was detected in the mid-infrared region. The optical conductivity spectrum under photoirradiation obtained from the Kramers-Kronig analyses of the reflectivity changes demonstrates a formation of a metallic state. This suggests that ferromagnetic spin arrangements occur within the time resolution (ca. 200 fs) through the double exchange interaction, resulting in an …
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…
We introduce an effective model for $e_g$ electrons to describe three-dimensional perovskite (La$_{1-x}$Sr$_{x}$MnO$_3$ and La$_{1-x}$Ca$_{x}$MnO$_3$) manganites and study the magnetic and orbital order on $4\times 4\times 4$ cluster using correlated wave functions. The model includes the kinetic energy, and on-site Coulomb interactions for $e_g$ electrons, antiferromagnetic superexchange interaction between $S=3/2$ core spins, and the coupling between $e_g$ electrons and Jahn-Teller modes. The model reproduces the experimentally observed magnetic order: ($i$) $A$-type antiferromagnetic phase …
Structural, magnetic and electric properties of a metal-ordered perovskite YBaMn2O6 have been studied by means of powder X-ray diffraction, DSC, magnetic susceptibility, and electric resistivity. It is found that this material undergoes a 1st order structural phase transition at Tc1=520 K, from a pseudo orthorhombic (monoclinic) phase to a pseudo tetragonal (monoclinic) one. Accompanied by this transition, the susceptibility exhibits a sharp drop, where ferromagnetic exchange interaction becomes antiferromagnetic. Furthermore, two more transitions, a metal-insulator transition at Tc2=480 K and…
Spin wave excitations were measured in the ferromagnetic phase of Nd$_{1/2}$Sr$_{1/2}$MnO$_{3}$ by neutron scattering. This compound is located in proximity to the A-type antiferromagnetic state, and it shows a clear anisotropy and anomalous softening of the spin wave excitations. The softening in the ferromagnetic phase is induced by the orbital ordering.
We discuss heat transport in hole-doped manganites, nickelates and cuprates for which real-space charge ordering has been observed. We survey the thermal transport response to charge order in the various materials and the associated structural modifications, particularly distortions of the metal-oxygen polyhedra associated with localized charge, that may be a principal source of phonon damping.
Charge-lattice fluctuations are observed in the layered perovskite manganite LaSr2Mn2O7 by Raman spectroscopy as high as 340 K and with decreasing temperature they become static and form a charge ordered (CO) phase below TCO=210 K. In the static regime, superlattice reflections are observed through neutron and x-ray diffraction with a propagation vector (h+1/4,k-1/4,l). Crystallographic analysis of the CO state demonstrates that the degree of charge and orbital ordering in this manganite is weaker than the charge ordering in three dimensional perovskite manganites. A TN=170K a type-A antiferro…
The low-temperature properties of the so-called ''charge ordered'' state in 50% doped perovskite manganites are described from the viewpoint of the magnetic spin ordering. In these systems, the zigzag antiferromagnetic ordering, combined with the double-exchange physics, effectively divides the whole sample into the one-dimensional ferromagnetic zigzag chains and results in the anisotropy of electronic properties. The electronic structure of one such chain is described by an effective 3$\times$3 Hamiltonian in the basis of Mn($3de_g$) orbitals. We treat this problem analytically and consider t…
Low as well as high-temperature electron and x-ray diffraction studies have been carried out on a rare-earth free B-site disordered electron-doped manganite SrMn0.875.Mo0.125O3-δ in the temperature range of 83K to 637K. These studies reveal the occurrence of strong charge ordering (CO) at room temperature in a pseudo tetragonally distorted perovskite phase with space-group Pmmm. Non integral modulation vector of 8.95 times along [-110] indicates a charge density wave type modulation. The CO phase with basic perovskite structure Pmmm transforms to a charge disorder cubic phase through a first o…
The orbital order-disorder transition temperature (T_OO) versus tolerance factor (t) plot switches from monotonic to non-monotonic beyond a doping level (x) ~ 10 atom% in a family of R(1-x)A(x)MnO3 systems(R = La, Pr, Nd; A = Ca, Sr; x = 0.0-0.2). T_OO reaches maximum at a 'doping-dependent' critical tolerance factor t_C(x) (for 0.1<x<0.2)at which the orthorhombic distortion (D) also maximizes. Such an observation reflects influence of charge carriers on both 'intrinsic' octahedral-site distortion and its bias on the orbital order in doped perovskite manganites and, thus, deviation from what h…
Magnon linewidth of La_1.2 Sr_1.8 Mn_2 O_7 near the Brillouin zone boundary is investigated from both theoretical and experimental points of view. Abrupt magnon broadening is ascribed to a strong magnon-phonon coupling. Magnon broadening observed in cubic perovskite manganites is also discussed.
We have investigated electrically-active magnetic excitations (electromagnons) in perovskite manganites with the $E$-type (up-up-down-down) spin structure by terahertz spectroscopy. Eu$_{1-x}$Y$_x$MnO$_3$ (0.1$\le x\le$1) and Y$_{1-y}$Lu$_y$MnO$_3$ (0$\le y\le$1) without magnetic $f$-moments, which host collinear sinusoidal, $A$-type, cycloidal, and $E$-type spin orders, are used to examine the systematics of possible electromagnons. Three-peak structures (23, 35, 45 cm$^{-1}$) of magnetic origin show up in the $E$-type phase with little composition ($y$) dependence of frequencies, making a co…
Pressure effects on the charge and spin dynamics in the bilayer manganite compounds $La_{2-2x}Sr_{1+2x}Mn_2O_7$ are studied theoretically by taking into account the orbital degrees of freedom. The orbital degrees are active in the layered crystal structure, and applied hydrostatic pressure stabilizes the $3d_{x^2-y^2}$ orbital in comparison with $3d_{3z^2-r^2}$. The change of the orbital states weakens the interlayer charge and spin couplings, and suppresses the three dimensional ferromagnetic transition. Numerical results, based on an effective Hamiltonian which includes the energy level diff…
Ultrasonic attenuation and phase velocity measurements have been carried out in the ferromagnetic perovskites La_{2/3}Ca_{1/3}MnO_3 and La_{2/3}Sr_{1/3}MnO_3. Data show that the transition at the Curie temperature, T_C, changes from first- to second-order as Sr replaces Ca in the perovskite. The compound with first-order transition shows also another transition at a temperature T* > T_C. We interpret the temperature window T_C < T < T* as a region of coexistence of a phase separated regime of metallic and insulating regions, in the line of recent theoretical proposals.
$^{139}$La- and $^{55}$Mn-NMR spectra demonstrate that the ground state of the A-site ordered perovskite manganite LaBaMn$_2$O$_6$ is a spatial mixture of the ferromagnetic (FM) and antiferromagnetic (AFI(CE)) regions, which are assigned to the metallic and the insulating charge ordered state, respectively. This exotic coexisting state appears below 200 K via a first-order-like formation of the AFI(CE) state inside the FM one. Mn spin-spin relaxation rate indicates that the FM region coexisting with the AFI(CE) one in LaBaMn$_2$O$_6$ is identical to the bulk FM phase of the disordered form La$…
Through a combination of neutron diffraction and Landau theory we describe the spin ordering in the ground state of the quadruple perovskite manganite CaMn7O12 - a magnetic multiferroic supporting an incommensurate orbital density wave that onsets above the magnetic ordering temperature, TN1 = 90 K. The multi-k magnetic structure in the ground state was found to be a nearly-constant-moment helix with modulated spin helicity, which oscillates in phase with the orbital occupancies on the Mn3+ sites via trilinear magneto-orbital coupling. Our phenomenological model also shows that, above TN2 = 48…
The origin of the spiral spin-order in perovskite multiferroic manganites $R$MnO$_{3}$ ($RE=$ Tb or Dy) is here investigated using a two $e_{\rm g}$-orbitals double-exchange model. Our main result is that the experimentally observed spiral phase can be stabilized by introducing a relatively weak next-nearest-neighbor superexchange coupling ($\sim10%$ of the nearest-neighbor superexchange). Moreover, the Jahn-Teller lattice distortion is also shown to be essential to obtain a realistic spiral period. Supporting our conclusions, the generic phase diagram of undoped perovskite manganites is obtai…
The magnetically ordered states of the A-site ordered perovskite manganites LaBaMn2O6 and YBaMn2O6 have been investigated by muon spin relaxation in zero external magnetic field. Our data reveal striking differences in the nature of the magnetically ordered state of these materials. For LaBaMn2O6, the muSR time-spectra in the ferromagnetic state below ~ 330 K reveal a strongly inhomogeneous phase, reminiscent of a Griffiths phase. Within this magnetically inhomogeneous phase, an antiferromagnetic state develops below 150 K, which displays well defined static internal magnetic fields, but reach…
Recent spectroscopic studies at terahertz frequencies for a variety of multiferroics endowed with both ferroelectric and magnetic orders have revealed the possible emergence of a new collective excitation, frequently referred to as electromagnon. It is magnetic origin, but becomes active in response to the electric field component of light. Here we give an overview on our recent advance in the terahertz time-domain spectroscopy of electromagnons or electric-dipole active magnetic resonances, focused on perovskite manganites--$R$MnO$_3$ ($R$ denotes rare-earth ions). The respective electric and…
Proximity to an orbital order with charge disorder state in optimally-doped \textit{RE}\textsubscript{5/8}Ca\textsubscript{3/8}MnO\textsubscript{3} perovskites
Structural behaviour of PbMn$_{7}$O$_{12}$ has been studied by high resolution synchrotron X-ray powder diffraction. This material belongs to a family of quadruple perovskite manganites that exhibit an incommensurate structural modulation associated with an orbital density wave. It has been found that the structural modulation in PbMn$_{7}$O$_{12}$ onsets at 294 K with the incommensurate propagation vector $\mathbf{k}_s=(0,0,\sim2.08)$. At 110 K another structural transition takes place where the propagation vector suddenly drops down to a \emph{quasi}-commensurate value $\mathbf{k}_s=(0,0,2.0…
We report a neutron powder diffraction study of $R$Mn$_7$O$_{12}$ quadruple perovskite manganites with $R$ = La, Ce, Nd, Sm, and Eu. We show that in all measured compounds concomitant magnetic ordering of the $A$ and $B$ manganese sublattices occurs on cooling below the N$\mathrm{\acute{e}}$el temperature. The respective magnetic structures are collinear, with one uncompensated Mn$^{3+}$ moment per formula unit as observed in bulk magnetisation measurements. We show that both LaMn$_7$O$_{12}$ and NdMn$_7$O$_{12}$ undergo a second magnetic phase transition at low temperature, which introduces a…
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 theory of resonant x-ray scattering in perovskite manganites is developed by applying the group theory to the correlation functions of the pseudospin operators for the orbital degree of freedom. It is shown that static and dynamical informations of the orbital state are directly obtained from the elastic, diffuse and inelastic scatterings due to the tensor character of the scattering factor. We propose that the interaction and its anisotropy between orbitals are directly identified by the intensity contour of the diffuse scattering in the momentum space.
In this contribution to the special issue on multiferroics we focus on multiferroicity driven by different forms of charge ordering. We will present the generic mechanisms by which charge ordering can induce ferroelectricity in magnetic systems. There is a number of specific classes of materials for which this is relevant. We will discuss in some detail $(i)$ perovskite manganites of the type (PrCa)MnO$_3$, $(ii)$ the complex and interesting situation in magnetite Fe$_3$O$_4$, $(iii)$ strongly ferroelectric frustrated LuFe$_2$O$_4$, $(iv)$ an example of a quasi one-dimensional organic system. …
Magnetic structures and the relationship between spin and charge-orbital orderings of an A-site ordered double-perovskite manganite SmBaMn2O6, an anticipated multiferroic material, were investigated by means of neutron diffraction. The spin arrangement in MnO2 planes perpendicular to the c axis is revealed to be the same as that in the A-site disordered half-doped manganites CE-type but the stacking pattern is found to be different displaying a unique twofold period. The temperature dependence of the superlattice magnetic and nuclear reflections clarifies that the antiferromagnetic spin orderi…
The phase diagram of quarter-hole-doped perovskite manganites is investigated using the doubleexchange model. An exotic striped type-II multiferroic phase, where 25% of the nearest-neighbor spin couplings are orthogonal to each other, is found in the narrow-bandwidth region. Comparing with the spiral-spin ordering phase of undoped manganites, the multiferroic Curie temperature of the new phase is estimated to be ~4 times higher, while the ferroelectric polarization is similar in magnitude. Our study provides a path for noncollinear spin multiferroics based on electronic self-organization, diff…
The specific heat of the perovskite manganite La0.78Pb0.22MnO3-d was measured from 0.5 to 25 K. The results yield values of the electronic density of states, the Debye temperature, and the spin-wave stiffness constant of the compound. The magnetic contribution was found to be consistent with the existence of a gap in the spin-wave spectrum, and a phonon term in T^5 was needed to fit the data.
We have investigated the electronic and magnetic properties of Co-doped Pr0.8Ca0.2MnO3 thin films using various spectroscopic techniques. X-ray absorption and hard x-ray photoemission spectroscopy revealed that the substituted Co ions are in the divalent state, resulting in hole doping on the Mn atoms. Studies of element-selective magnetic properties by x-ray magnetic circular dichroism found a large orbital magnetic moment for the Co ions. These spectroscopic studies reveal that the substituted Co ions play several roles of hole doping for Mn, ferromagnetic superexchange coupling between the …
Results of LSDA and LSDA+U calculations of the electronic structure and magnetic configurations of the 50% hole-doped pseudocubic perovskite La0.5Sr0.5MnO3 and double layered LaSr2Mn2O7 are presented. We demonstrate that the on-site Coulomb correlation (U) of Mn d electrons has a very different influence on the (i) band formations, (ii) magnetic ground states, (iii) interlayer exchange interactions, and (iv) anisotropy of the electrical transport in these two manganites. A possible reason why the LSDA failures in predicting observed magnetic and transport properties of the double layered compo…
In this paper, we present the spin-phonon coupling and dielectric response of nano-crystalline Pr$_2$CoMnO$_6$ employing Raman and dielectric spectroscopic study. Pr$_2$CoMnO$_6$ is a manganite compound , it undergoes a paramagnetic to ferromagnetic (PM-FM) phase transition around $T_c$ $\sim$172 K. Temperature-dependent Raman scattering experiment is carried out across $T_c$ to study the spin-phonon behavior in this material. The results from Raman study reveal an obvious softening of the phonon mode involving stretching vibrations of the (Co/Mn)O$_6$ octahedra in ferromagnetic temperature re…
