We present a comprehensive theory of the temperature- and disorder-dependence of half-metallic ferrimagnetism in the double perovskite Sr$_2$FeMoO$_6$ (SFMO) with $T_c$ above room temperature. We show that the magnetization $M(T)$ and conduction electron polarization $P(T)$ are both proportional to the magnetization $M_S(T)$ of localized Fe spins. We derive and validate an effective spin Hamiltonian, amenable to large-scale three-dimensional simulations. We show how $M(T)$ and $T_c$ are affected by disorder, ubiquitous in these materials. We suggest a way to enhance $T_c$ in SFMO without sacrificing polarization.
The magnetic properties of GdBaMn_{2}O_{5.0}, which exhibits charge ordering, are studied from 2 to 400 K using single crystals. In a small magnetic field applied along the easy axis, the magnetization M shows a temperature-induced reversal which is sometimes found in ferrimagnets. In a large magnetic field, on the other hand, a sharp change in the slope of M(T) coming from an unusual turnabout of the magnetization of the Mn sublattices is observed. Those observations are essentially explained by a molecular field theory which highlights the role of delicate magnetic interactions between Gd^{3…
We show that a superstructure of antiferromagnetically interacting Fe$^{3+}$ ($S=5/2$) ions in double perovskites AFe$_{1/2}$M$_{1/2}$O$_{3}$ exhibits a ferrimagnetic ordering below $T_{fe} \approx 5.6J_1$ ($J_1/k_B \sim 50$~K), which is close to room temperature. Small clusters of the same structure exhibit a superparamagnetic behavior at $T \lesssim T_{fe}$. The possibility of formation of such clusters explains the room-temperature (superpara)magnetism in 3$d$-metal based oxides.
The non-stoichiometric double perovskite oxide La2Ni1.19Os0.81O6 was synthesized by solid state reaction and its crystal and magnetic structures were investigated by powder x-ray and neutron diffraction. La2Ni1.19Os0.81O6 crystallizes in the monoclinic double perovskite structure (general formula A2BB'O6) with space group P21/n, where the B site is fully occupied by Ni and the B' site by 19 % Ni and 81 % Os atoms. Using x-ray absorption spectroscopy an Os4.5+ oxidation state was established, suggesting presence of about 50 % paramagnetic Os5+ (5d3, S = 3/2) and 50 % non-magnetic Os4+ (5d4, Jef…
Spin-reorientation phase transitions that involve the rotation of a crystal$'$s magnetization have been well characterized in distorted-perovskite oxides such as the orthoferrites. In these systems spin reorientation occurs due to competing rare-earth and transition metal anisotropies coupled via $f$-$d$ exchange. Here, we demonstrate an alternative paradigm for spin reorientation in distorted perovskites. We show that the $R_2\mathrm{CuMnMn_4O_{12}}$ (R = Y or Dy) triple A-site columnar-ordered quadruple perovskites have three ordered magnetic phases and up to two spin-reorientation phase tra…
Using density functional calculations, we find that the newly synthesized Ca$_2$FeOsO$_6$ has the high-spin Fe$^{3+}$ ($3d^5$)-Os$^{5+}$ ($5d^3$) state. The octahedral Os$^{5+}$ ion has a large intrinsic exchange splitting, and its $t_{2g\uparrow}^3$ configuration makes the spin-orbit coupling ineffective. Moreover, there is a strong antiferromagnetic (AF) coupling between the neighboring Fe$^{3+}$ ($S$ = 5/2) and Os$^{5+}$ ($S$ = -3/2), but the AF couplings within both the fcc Fe$^{3+}$ and Os$^{5+}$ sublattices are one order of magnitude weaker. Therefore, a magnetic frustration is suppresse…
The high temperature ferromagnetism in Sr3YCo4O10+delta perovskite, whose origin has been the subject of a considerable debate, has been studied by neutron powder diffraction and synchrotron X-ray diffraction measurements. Oxygen vacancy ordering creates a complex pattern of zigzag stripes in the oxygen-deficient CoO4+delta layers, where the Co ions are found in three distinct coordinations. The symmetry of this unprecedented structural modulation, in conjunction with the existence of different Co spin states, provide a straightforward explanation for the appearance of ferrimagnetism. A model …
Room-temperature ferrimagnetism was discovered for the anti-site-disordered perovskite Ca2MnOsO6 with Tc = 305 K. Ca2MnOsO6 crystallizes into an orthorhombic structure with a space group of Pnma, in which Mn and Os share the oxygen-coordinated-octahedral site at an equal ratio without a noticeable ordered arrangement. The material is electrically semiconducting with variable-range-hopping behavior. X-ray absorption spectroscopy confirmed the trivalent state of the Mn and the pentavalent state of the Os. X-ray magnetic circular dichroism spectroscopy reveals that the Mn and Os magnetic moments …
Titanates with the perovskite structure, including ferroelectrics (e.g., BaTiO$_3$) and ferromagnetic ones (e.g., YTiO$_3$), are important functional materials. Recent theoretical studies predicted multiferroic states in strained EuTiO$_3$ and titanate superlattices, the former of which has already been experimental confirmed. Here, a first-principles calculation is performed to investigate the structural, magnetic, and electronic properties of Y half-substituted LaTiO3. Our results reveal that the magnetism of Y$_{0.5}$La$_{0.5}$TiO$_3$ sensitively depends on its structural details because of…
The Slater-Pauling rule states that L21 Heusler compounds with 24 valence electrons do never exhibit a total spin magnetic moment. In case of strongly localized magnetic moments at one of the atoms (here Mn) they will exhibit a fully compensated half-metallic ferrimagnetic state instead, in particular, when symmetry does not allow for antiferromagnetic order. With aid of magnetic and anomalous Hall effect measurements it is experimentally demonstrated that Mn1.5V0.5FeAl follows such a scenario. The ferrimagnetic state is tuned by the composition. A small residual magnetization, that arises due…
Recently, in the seemingly narrow gap insulating NiCrO$_3$ with the trigonally distorted (R-3c) perovskite-like structure, a compensated half-metal (CHM) is predicted, as applying a modest pressure. Using ab initio calculations including both Coulomb correlations and spin-orbit coupling (SOC), we investigate the as-yet-unsynthesized PdCrO$_3$, isostructural and isovalent to NiCrO$_3$. Upon applying the on-site Coulomb repulsion $U$ to both Pd and Cr ions, the Cr spin moment is precisely compensated with the antialigned spin moments of Pd and oxygens. Coincidentally only one spin channel remain…
We present an interacting model for the electronic and magnetic behavior of a strained $(001)$ atomic layer of Sr$_2$FeMoO$_6,$ which shows room-temperature ferrimagnetism and magnetoresistance with potential spintronics application in the bulk. We find that the strong spin-orbit coupling in the molybdenum 4$d$ shell gives rise to a robust ferrimagnetic state with an emergent spin-polarized electronic structure consisting of flat bands and four massive or massless Dirac dispersions. Based on the spin-wave theory, we demonstrate that the magnetic order remains intact for a wide range of doping,…
In the search for new spintronic materials with high spin-polarization at room-temperature, we have synthesized an osmium based double perovskite with a Curie-temperature of 725 K. Our combined experimental results confirm the existence of a sizable induced magnetic moment at the Os site, supported by band-structure calculations in agreement with a proposed kinetic energy driven mechanism of ferrimagnetism in these compounds. The intriguing property of Sr2CrOsO6 is that it is at the endpoint of a metal-insulator transition due to 5d band filling, and at the same time ferrimagnetism and high-sp…
We studied structural and magnetic properties of a series of insulating double perovskite compounds, La$_{2-x}$Sr$_{x}$CuRuO$_{6}$ (0 $\le$ x $\le$ 1), representing doping via \textit{A}-site substitution. The end members La$_{2}$CuRuO$_{6}$ and LaSrCuRuO$_{6}$ form in monoclinic structure while the intermediate Sr doped compounds stabilise in triclinic structure. The Cu and Ru ions sit on alternate B-sites of the perovskite lattice with $\sim$15% anti-site defects in the undoped sample while the Sr doped samples show a tendency to higher ordering at B-sites. The undoped (x = 0) compound shows…
The double perovskite material \SFMO has the rare and desirable combination of a half-metallic ground state with 100% spin polarization and ferrimagnetic \Tc$\simeq 420$K, well above room temperature. In this two-part paper, we present a comprehensive theoretical study of the magnetic and electronic properties of half metallic double perovskites. In this paper we present exact diagonalization calculations of the "fast" Mo electronic degrees coupled to "slow" Fe core spin fluctuations treated by classical Monte Carlo techniques. From the temperature dependence of the spin-resolved density of st…
Double perovskites like Sr$_2$FeMoO$_6$ are materials with half-metallic ground states and ferrimagnetic T$_{\rm{c}}$'s well above room temperature. This paper is the second of our comprehensive theory for half metallic double perovskites. Here we derive an effective Hamiltonian for the Fe core spins by "integrating out" the itinerant Mo electrons and obtain an unusual double square-root form of the spin-spin interaction. We validate the classical spin Hamiltonian by comparing its results with those of the full quantum treatment presented in the companion paper "Theory of Half-Metallic Double …
We present a microscopic theory of carrier-induced ferrimagnetism in metallic double perovskite compounds such as ${\rm Sr}_{2}{\rm FeMoO}_{6}$ and ${\rm Sr}_{2}{\rm FeReO}_{6}$ which have recently attracted intense interest for their possible applications to magnetotransport devices. The theory is based on an effective "Kondo-like" Hamiltonian treated here within the large-$S$ expansion. We find that depending on the value of the carrier density the ground state is either a ferrimagnet or a layered antiferromagnet. The ferrimagnetic state has a robust half-metallic electronic structure. The t…
We present a powder inelastic neutron scattering study of magnetic excitations in Ba$_2$FeReO$_6$, a member of the double perovskite family of materials which exhibit half-metallic behavior and high Curie temperatures. We find clear evidence of two well-defined dispersing magnetic modes in its low temperature ferrimagnetic state. We develop a local moment model, which incorporates the interaction of Fe spins with spin-orbit locked magnetic moments on Re, and show that this captures our experimental observations. Our study further opens up double perovskites as model systems to explore the inte…
Based on the theoretical exploration of electronic structures, we propose that the ordered double perovskites LaAVRuO$_6$ and LaVO$_3$/ARuO$_3$ (001) superlattice (A = Ca, Sr and Ba) are strong candidates for half-metallic (HM) antiferromagnets (AFMs). %LaAVRuO$_6$ and LaVO$_3$/ARuO$_3$ have the %100% spin polarizations at the Fermi level but with zero %total magnetic moments. We have shown that the HM-AFM nature in LaAVRuO$_6$ is very robust regardless of (i) divalent ion replacement at A-sites, (ii) oxygen site relaxation, (iii) the inclusion of the Coulomb correlation, and (iv) cation disor…
We report on a study of charge transport in EuTiO$_{3-δ}$ single crystals with carrier density tuned across several orders of magnitude. Comparing this system with other quasi-cubic perovskites, in particular strontium titanate, we draw a comprehensive picture of metal-insulator transition and dilute metallicity in this $AB$O$_3$ family. Because of a lower electric permittivity, the metal-insulator transition in EuTiO$_{3-δ}$ occurs at higher carrier densities compared to SrTiO$_3$. At low temperature, a distinct $T^2$ resistivity is visible. Its prefactor $A$ smoothly decreases with increasin…
Using the first-principles density functional approach, we investigate Ca$_2$FeOsO$_6$, a material of double perovskite structure synthesized recently. According to the calculations, Ca$_2$FeOsO$_6$ is a ferrimagnetic Mott-insulator influenced by the cooperative effect of spin-orbit coupling (SOC) and Coulomb interactions of Fe-3$d$ and Os-5$d$ electrons, as well as the crystal field. When Fe is replaced with Ni, the system exhibits half metallic (HM) states desirable for spintronic applications. In [Ca$_2$Fe$_{1-x}$Ni$_x$OsO$_6$]$_2$, HM ferrimagnetism is observed with $μ_{\rm tot}=2μ_{\rm B}…
A previously unreported Pb-based perovskite PbMoO$_3$ is obtained by high-pressure and high-temperature synthesis. This material crystallizes in the $Pm\bar{3}m$ cubic structure at room temperature, making it distinct from typical Pb-based perovskite oxides with a structural distortion. PbMoO$_3$ exhibits a metallic behavior down to 0.1 K with an unusual $T$-sub linear dependence of the electrical resistivity. Moreover, a large specific heat is observed at low temperatures accompanied by a peak in $C_P/T^3$ around 10 K, in marked contrast to the isostructural metallic system SrMoO$_3$. These t…
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…
The new perovskite cuprate material Sr$_{8}$CaRe$_{3}$Cu$_{4}$O$_{24}$, which behaves ferrimagnetically and shows an unusually high Curie temperature ($T_c \sim$ 440 K), is found from density-functional theory calculation to display several surprising properties after hole doping or chemical substitution: (1) Half metal (HM) is realized by replacing Re with W or Mo while $T_c$ remains high; (2) hole-doped Sr$_{8}$CaRe$_{3}$Cu$_{4}$O$_{24}$ is also HM with high $T_c$. Moreover, we find that the O atoms will carry a large magnetic moment after hole doping, which is in sharp contrast with the gen…
The zero-field conductivities ($σ$) of the polycrystaline title materials, are governed by inter-grain transport. In the majority of cases their $σ$(T) can be described by the "fluctuation induced tunneling" model. Analysis of the results in terms of this model reveals two remarkable features: 1. For \emph{all} Sr$_2$FeMoO$_6$ samples of various microstructures, the tunneling constant (barrier width $\times$ inverse decay-length of the wave-function) is $\sim$ 2, indicating the existence of an intrinsic insulating boundary layer with a well defined electronic (and magnetic) structure. 2. The t…
Using ab initio calculations, we have investigated a cubic perovskite BaOsO3 and a few related compounds that have been synthesized recently and formally have a metallic d^4 configuration. In BaOsO3, which shows obvious 3-dimensional fermiology, a nonmagnetism is induced by a large spin-orbit coupling (SOC), which is precisely equal to an exchange splitting ~0.4 eV of the $t_{2g}$ manifold. However, the inclusion of on-site Coulomb repulsion as small as $U^c$~1.2 eV, only 1/3 of the $t_{2g}$ bandwidth, leads to the emergence of a spin-ordered moment, indicating that this system is on the verge…
he structural, transport, magnetic and optical properties of the double perovskite $A_2$CrWO$_6$ with $A=\text{Sr, Ba, Ca}$ have been studied. By varying the alkaline earth ion on the $A$ site, the influence of steric effects on the Curie temperature $T_C$ and the saturation magnetization has been determined. A maximum $T_C=458$ K was found for Sr$_2$CrWO$_6$ having an almost undistorted perovskite structure with a tolerance factor $f\simeq 1$. For Ca$_2$CrWO$_6$ and Ba$_2$CrWO$_6$ structural changes result in a strong reduction of $T_C$. Our study strongly suggests that for the double perovsk…
The two-dimensional layered perovskite Sr2IrO4 was proposed to be a spin-orbit Mott insulator, where the effect of Hubbard interaction is amplified on a narrow J_{eff} = 1/2 band due to strong spin-orbit coupling. On the other hand, the three-dimensional orthorhombic perovskite (Pbnm) SrIrO3 remains metallic. To understand the physical origin of the metallic state and possible transitions to insulating phases, we construct a tight-binding model for SrIrO3. The band structure possesses a line node made of J_{eff} = 1/2 bands below the Fermi level. As a consequence, instability towards magnetic …
Several double perovskite materials of the form A_2BB'O_6 exhibit high ferromagnetic T_c, and significant low field magnetoresistance. They are also a candidate source of spin polarized electrons. The potential usefulness of these materials is, however, frustrated by mislocation of the B and B' ions, which do not organise themselves in the ideal alternating structure. The result is a strong dependence of physical properties on preparative conditions, reducing the magnetization and destroying the half-metallicity. We provide the first results on the impact of spatially correlated antisite disor…
We have deployed density functional theory, Wannier function analysis and mean-field calculations to investigate the double-double perovskite compound CaMnCrSbO_{6}. The crystallographically non-equivalent Mn atoms in the unit cell have tetrahedral and planar oxygen coordinations (labelled as Mn(1) and Mn(2)), while the Cr atom is in the centre of distorted oxygen octahedron. While the bulk magnetization and neutron diffraction suggest a simpler ferrimagnetic order (T_C=49 K) between Mn2+ and Cr3+ spins, the exchange interactions are more complex than that expected from a two sublattice magnet…
We analyzed the possible magnetic and orbital orderings of double perovskites, using a simple extension of the double exchange model well suited for these compounds. Orbital ordering is favored by the on site repulsion at the Fe ions. We obtain a rich phase diagram, including ferri- and antiferromagnetic phases, which can, in turn, be metallic or insulating, depending on the existence of orbital order.
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 …
Using first principles calculations, we investigate the electronic and magnetic properties of the trigonally distorted (R-3c) perovskite-derived NiCrO$_3$. Within the local spin density approximation (LSDA), our calculations show that this system is an exactly compensated half-metal (CHM). The local spin moments of Cr 2.04, and antialigned Ni -1.41 and three oxygens -0.63 (in the units of $μ_B$), indicate high spin S=3/2 Cr$^{3+}$ and S=3/2 (NiO$_3$)$^{3-}$ units. Considering reasonable values of the on-site Coulomb repulsion U on both Ni and Cr ions with LDA+U approach, this system becomes an…
Half-metallic ferromagnets show 100% spin-polarization at the Fermi level and are ideal candidates for spintronic applications. Despite the extensive research in the field, very few materials have been discovered so far. Here we present results of electronic band structure calculations based on density functional theory and extensive physical-property measurements for Fe3Se4 revealing signatures of half-metallicity. The spin-polarized electronic band structure calculations predict half-metallic ferrimagnetism for Fe3Se4. The electrical resistivity follows exponentially suppressed electron-magn…
Taking into account Goodenough's superexchange rules, including both full structural relaxation and spin-orbit coupling, and checking strong correlation effects, we look for compensated half metals within the class of oxide double perovskites materials. Identifying likely half metallic (or half semimetallic) antiferromagnets, the full complications including orbital magnetism are included in order to arrive at realistic predictions of designed magnetic compounds with (near) vanishing net moment. After sorting through several candidates that have not been considered previously, two materials, K…
We have investigated the structure and electronic properties of ferrimagnetic double perovskites, A2FeReO6 (A= Ca, Sr, Ba). The A=Ba phase is cubic (Fm3m) and metallic, while the A=Ca phase is monoclinic (P21/n) and nonmetallic. 57Fe Mossbauer spectroscopy shows that iron is present mainly in the high-spin (S=5/2) Fe3+ state in the Ca compound, while it occurs in an intermediate state between high-spin Fe2+ and Fe3+ in the Ba compound. It is argued that a direct Re t2g - Re t2g interaction is the main cause for the metallic character of the Ba compound; the high covalency of Ca-O bonds and the…
A remarkable hardening (~ 30 cm-1) of the normal mode of vibration associated with the symmetric stretching of the oxygen octahedra for the Ba2FeReO6 and Sr2CrReO6 double perovskites is observed below the corresponding magnetic ordering temperatures. The very large magnitude of this effect and its absence for the anti-symmetric stretching mode provide evidence against a conventional spin-phonon coupling mechanism. Our observations are consistent with a collective excitation formed by the combination of the vibrational mode with oscillations of local Fe or Cr 3d and Re 5d occupations and spin m…
We report a study of the magnetoresistance (MR) of the metallic perovskite oxide LaNiO$_{3-δ}$ as a function of the oxygen stoichiometry $δ$ ($δ\leq$ 0.14), magnetic field (H $\leq 6T$) and temperature (1.5K $\leq $ T $\leq $ 25K). We find a strong dependence of the nature of MR on the oxygen stoichiometry. The MR at low temperatures change from positive to negative as the sample becomes more oxygen deficient (i.e, $δ$ increases). Some of the samples which are more resistive, show a resistivity minima at $T_{min}$ $\approx$ 20K. We find that in these samples the MR is positive at T > $T_{min}$…
We demonstrate in a simple model the surprising result that turning on an on-site Coulomb interaction U in a doped band insulator leads to the formation of a half-metallic state. In the undoped system, we show that increasing U leads to a first order transition between a paramagnetic, band insulator and an antiferomagnetic Mott insulator at a finite value U_{AF}. Upon doping, the system exhibits half metallic ferrimagnetism over a wide range of doping and interaction strengths on either side of U_{AF}. Our results, based on dynamical mean field theory, suggest a novel route to half-metallic be…
We present the self-interaction corrected local spin density (SIC-LSD) electronic structure and total energy calculations, leading also to valencies of the ground state configurations, for the half-metallic double perovskites such as Sr$_{2}$FeMoO$_{6}$, Ba$_{2}$FeMoO$_{6}$, Ca$_{2}$FeMoO$_{6}$, and Ca$_{2}$FeReO$_{6}$. We conclude that the Fe and Mo (or Re) spin magnetic moments are anti-parallel aligned, and the magnitude of the hybridization induced moment on Mo does not vary much between the different compounds. The hybridization spin magnetic moment on Re is of the order of -1.1 $μ_{B}$, …
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 study the effect of Coulomb interactions in transition metal oxides junctions. In this paper we analyze charge transfer at the interface of a three layer ferromagnetic-paramagnetic-ferromagnetic metallic oxide system. We choose a charge model considering a few atomic planes within each layer and obtain results for the magnetic coupling between the ferromagnetic layers. For large number of planes in the paramagnetic spacer we find that the coupling oscillates with the same period as in RKKY but the amplitude is sensitive to the Coulomb energy. At small spacer thickness however, large differe…
We report investigations of the structural, magnetic, electrical transport and thermal properties of five compositions of the metallic perovskite GdRh$_3$C$_{1-x}$B$_x$ ($0.00 \le x \le 1.00$). Our results show that all the five compositions undergo magnetic ordering at low temperatures, but the nature of the ordered state is significantly different in the carbon- and the boron-rich compositions, where the former shows signatures of an amplitude-modulated magnetic structure and the latter exhibits evidences of an equal-moment incommensurate antiferromagnetic ordering. We also observe a remarka…
We consider a model of the double perovskite Ba2FeReO6, a room temperature ferrimagnet with correlated and spin-orbit coupled Re t2g electrons moving in the background of Fe moments stabilized by Hund's coupling. We show that for such 3d/5d double perovskites, strong correlations on the 5d-element (Re) are essential in driving a half-metallic ground state. Incorporating both strong spin-orbit coupling and the Hubbard repulsion on Re leads to a band structure consistent with ab initio calculations. Using our model, we find a large spin polarization at the Fermi level, and obtain a semi-quantita…
Newly synthesized perovskite NaOsO3 shows Curie-Weiss metallic nature at high temperature and suddenly goes into an antiferromagnetically insulating state at 410 K on cooling. Electronic specific heat at the low temperature limit is absent, indicating that the band gap fully opens. In situ observation in electron microscopy undetected any lattice anomalies in the vicinity of the transition temperature. It is most likely that the antiferromagnetic correlation plays an essential role of the gap opening.
We discuss Mott insulating and metallic phases of a model with $e_g$ orbital degeneracy to understand physics of Mn perovskite compounds. Quantum Monte Carlo and Lanczos diagonalization results are discussed in this model. To reproduce experimental results on charge gap and Jahn-Teller distortions, we show that a synergy between the strong correlation effects and the Jahn-Teller coupling is important. The incoherent charge dynamics and strong charge fluctuations are characteristic of the metallic phase accompanied with critical enhancement of short-ranged orbital correlation near the insulator…
We have measured the photoemission spectra of Nd$_{1-x}$Sm$_{x}$NiO$_{3}$, where the metal-insulator transition and the Néel ordering occur at the same temperature for $x \lesssim 0.4$ and the metal-insulator transition temperature ($T_{MI}$) is higher than the Néel temperature for $x \gtrsim 0.4$. For $x \le 0.4$, the spectral intensity at the Fermi level is high in the metallic phase above $T_{MI}$ and gradually decreases with cooling in the insulating phase below $T_{MI}$ while for $x > 0.4$ it shows a pseudogap-like behavior above $T_{MI}$ and further diminishes below $T_{MI}$. The results…
Mesoscopic (500-2000 Angstrom) and microscopic (5-20 Angstrom) phase segregation with temperature and magnetic field was studied in the model manganite Pr0.7Ca0.3MnO3 by high-resolution neutron diffraction and inelastic neutron scattering. Intra-granular strain-driven mesoscopic segregation between two insulating phases, one of which is charge ordered (CO), sets in below the CO temperature in zero field. The CO phase orders antiferromagnetically, while the other insulating phase shows spin-glass behavior. After field-induced metallization, the CO phase coexists with a ferromagnetic metallic ph…
We have studied the electronic and magnetic properties of double perovskites Gd2MgIrO6 by first-principles density functional theory (DFT). Based on the DFT calculations, Gd2MgIrO6 is found to have a ferromagnetic (FM) ground state. The material undergo half-metallic ferromagnets to Mott-Hubbard insulator transition which happens due to strong correlation in Gd-4f and Ir-5d states. Our results shows that the 5d electrons of Ir hybridize strongly with O-2p states near the Fermi level giving rise to the insulating state of Gd2MgIrO6. Our study suggests that the enhanced magnetic moment is a resu…
Single crystals of the perovskite-type $3d^{1}$ metallic alloy system Ca$_{1-x}$Sr$_x$VO$_3$ were synthesized in order to investigate metallic properties near the Mott transition. The substitution of a Ca$^{2+}$ ion for a Sr$^{2+}$ ion reduces the band width $W$ due to a buckling of the V-O-V bond angle from $\sim180^\circ$ for SrVO$_3$ to $\sim160^\circ$ for CaVO$_3$. Thus, the value of $W$ can be systematically controlled without changing the number of electrons making Ca$_{1-x}$Sr$_x$VO$_3$: one of the most ideal systems for studying band-width effects. The Sommerfeld-Wilson's ratio ($\sime…
Synchrotron X-ray diffraction patterns were measured and analyzed for a polycrystalline sample of the room-temperature ferromagnet Sr3.12Er0.88Co4O10.5 from 300 to 650 K, from which two structural phase transitions were found to occur successively. The higher-temperature transition at 509 K is driven by ordering of the oxygen vacancies, which is closely related to the metallic state at high temperatures. The lower-temperature transition at 360 K is of first order, at which the ferromagnetic state suddenly appears with exhibiting a jump in magnetization and resistivity. Based on the refined str…
In the family of double perovskites, colossal magnetoresistance (CMR) has been so far observed only in half-metallic ferrimagnets such as the known case Sr$_2$FeMoO$_6$ where it has been assigned to the tunneling MR at grain boundaries due to the half-metallic nature. Here we report a new material-Tl$_2$NiMnO$_6$, a relatively ordered double perovskite stablized by the high pressure and high temperature synthesis-showing CMR in the vicinity of its Curie temperature. We explain the origin of such effect with neutron diffraction experiment and electronic structure calculations that reveal the ma…
We have investigated the electronic structure of meta-stable perovskite Ca1-xSrxIrO3 (x = 0, 0.5, and 1) thin films using transport measurements, optical spectroscopy, and first-principles calculations. We artificially fabricated the perovskite phase of Ca1-xSrxIrO3, which has a hexagonal or post perovskite crystal structure in bulk form, by growing epitaxial thin films on perovskite GdScO3 substrates using epi-stabilization technique. The transport properties of the perovskite Ca1-xSrxIrO3 films systematically changed from nearly insulating (or semi-metallic) for x = 0 to bad metallic for x =…
A systematic study of (A,A')2FeMoO6 (A,A'=Ca, Sr, Ba) ferromagnetic oxides with double perovskite structure has been performed using 95,97Mo and 57Fe NMR spectroscopy. These oxides are isoelectronic but have substantially different Curie temperatures. The NMR analysis provides clear evidence that the magnetic moment at Mo sites is not constant but varies sensitively with the ionic size of the alkaline ions. The 95,97Mo frequency, and thus the electronic charge at Mo ions, is found to be smaller in Ba and Ca than in Sr-based oxides. The charge release from Mo sites is accompanied by an uptake a…
Strong spin-orbit coupled 5d transition metal based ABO3 oxides, especially iridates, allow tuning parameters in the phase diagram and may demonstrate important functionalities, for example, by means of strain effects and symmetry-breaking, because of the interplay between the Coulomb interactions and strong spin-orbit coupling. Here, we have epitaxially stabilized high quality thin films of perovskite (Pv) CaIrO3. Film on the best lattice-matched substrate shows semi-metal-like characteristics. Intriguingly, imposing tensile or compressive strain on the film by altering the underlying lattice…
We have prepared crystallographically ordered and disorder specimens of the double perovskite, Sr$_2$FeMoO$_6$ and investigated their magnetoresistance behaviour. The extent of ordering between the Fe and Mo sites in the two samples is determined by Rietveld analysis of powder x-ray diffraction patterns and reconfirmed by Mössbauer studies. While the ordered sample exhibits the sharp low-field response, followed by moderate changes in the magnetoresistance at higher fields, the disordered sample is characterised by the absence of the spectacular low-field response. We argue that the low field …
We report here on the electronic structure of electron-doped half-metallic ferromagnetic perovskites such Sr$_{2-x}$La$_x$FeMoO$_6$ ($x$=0-0.6) as obtained from high-resolved valence-band photoemission spectroscopy (PES). By comparing the PES spectra with band structure calculations, a distinctive peak at the Fermi level (E$_F$) with predominantly (Fe+Mo) t$_{2g}^\downarrow$ character has been evidenced for all samples, irrespectively of the $x$ values investigated. Moreover, we show that the electron doping due to the La substitution provides selectively delocalized carriers to the t$_{2g}^\d…
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 investigate the unusual phase transitions in SrRuO$_{3}$ and Sr$_{0.5}$Ca$_{0.5}$Ru$_{1-x}$Cr$_{x}$O$_{3}$ (x=0,0.05 and 0.1) employing x-ray diffraction, resistivity, magnetic studies and x-ray photoemission spectroscopy. Our results show the compounds undergo crossover from $itinerant$ ferromagnetism to $localised$ ferromagnetism. The combined studies suggests Ru and Cr to be in 4+ valence state. A Griffith phase and an enhancement in Curie temperature (Tc) from 38 K to 107 K is observed with Cr doping. A shift in the chemical potential towards the valence band is observed with Cr doping.…
We construct an effective Hamiltonian for the motion of electrons among the transition metal ions of ordered double perovskites like Sr2FeMoO6. in which strong intra-atomic Coulomb repulsion U is present in only one of the inequivalent transition metal sites. Using a slave-boson formalism, we construct a phase diagram which describes a charge transfer transition between insulating and metallic behavior as the parameters of the model are changed. The parameters for Sr2FeMoO6 are estimated from first-principles calculations and a transition to the insulating state with negative pressure is obtai…
