Magnetic structures of metastable perovskites ScCrO3, InCrO3 and TlCrO3, stabilized under high-pressure and high-temperature conditions, have been studied by neutron powder diffraction. Similar to the other orthochromites LnCrO3 (Ln=lanthanide or Y), these materials crystallize into the orthorhombic structure with Pnma10 symmetry. The spin configuration of the metastable perovskites has been found to be C-type, contrasting with the G-type structure usually observed in LnCrO3. First-principles calculations demonstrate that the Ctype structure found in ScCrO3 and InCrO3 is attributed to a ferromagnetic (FM) nearest-neighbor interaction, while in TlCrO3, this type of magnetic ordering is stabilized by a strong next-nearest-neighbor antiferromagnetic (AFM) exchange. The spins in the C-type magnetic structure line up along the orthorhombic b-axis, yielding the Pnma magnetic symmetry. The dominant mechanism controlling this spin direction has been concluded to be the single ion anisotropy imposed by a uniaxial distortion of CrO6 octahedra.
The GdFeO$_{3}$-type perovskite CaCoO$_{3}$ has been successfully synthesized by high-pressure oxygen annealing for the oxygen deficient perovskite. A detailed structural analysis based on synchrotron X-ray diffraction data and a thermogravimetric analysis show that the valence of Co is +4 and the sample is free from oxygen deficiency. This compound shows an antiferromagnetic ordering at 95 K, which has presumably helical spin arrangement, with keeping the incoherent metallic state down to the lowest temperature. This work demonstrates that the Co$^{4+}$-perovskite oxides exhibit a variety of …
We report the observation of unusual exchange bias phenomena in the doped perovskite cobaltites La_{1-x}Sr_{x}CoO_{3} (x = 0.15, 0.18, and 0.30) in which a spontaneous phase separation into ferromagnetic clusters embedded in a non-ferromagnetic matrix occurs. When the La_{1-x}Sr_{x}CoO_{3} samples are cooled in a static magnetic field through a freezing temperature, the magnetization hysteresis loops exhibit exchange bias, i.e., the loops shift to the negative field and the magnetization becomes asymmetric. Moreover, exchange bias disappears when the measuring magnetic field is high enough. Th…
Understanding the structural underpinnings of magnetism is of great fundamental and practical interest. Se_{1-x}Te_{x}CuO_{3} alloys are model systems for the study of this question, as composition-induced structural changes control their magnetic interactions. Our work reveals that this structural tuning is associated with the position of the supposedly dummy atoms Se and Te relative to the super-exchange (SE) Cu--O--Cu paths, and not with the SE angles as previously thought. We use density functional theory, tight-binding, and exact diagonalization methods to unveil the cause of this surpris…
While double perovskites A2BB'O6, if ordered, usually form a rock-salt-type structure with a checkerboard B/B' ordering, it is surprising that Ca2FeMnO6 has alternate FeO2 and MnO2 layers in its perovskite structure. Here we demonstrate, using density functional calculations, that this unusual layered ordering facilitates, and is largely helped by, the Fe3+-Fe5+ charge disproportionation (CD) of the formal Fe4+ ions, which would otherwise be frustrated in the common rock salt structure. To further verify the important role of the CD for stabilization of this layered ordering, we carry out a co…
Electronic transport has been investigated for strong spin-orbit coupled perovskite SrIrO3 thin films grown at various substrate temperatures. The electronic transport of the SrIrO3 films is found to be very sensitive to the growth parameters; in particular, the film can either be a metal or an insulator depending upon the substrate growth temperature. While all the metallic films show unusual sublinear temperature dependent non-Fermi liquid behaviors in resistivity, the insulating film grown at a higher temperature stands out for its inhomogeneous Ir distribution, as analyzed by secondary ion…
Given the consensus that pressure improves cation order in most of known materials, a discovery of pressure-induced disorder could require reconsideration of order-disorder transition in solid state physics/chemistry and geophysics. Double perovskites Y2CoIrO6 and Y2CoRuO6 synthesized at ambient pressure show B-site order, while the polymorphs synthesized at 6 and 15 GPa are partially-ordered and disordered respectively. With the decrease of ordering degrees, the lattices are shrunken and the crystal structures alter from monoclinic to orthorhombic symmetry. Correspondingly, long-range ferrima…
BaRuO3 having five different crystal structures has been synthesized by varying the pressure while sintering. Contrary to the other phases being nonmagnetic, the cubic perovskite phase synthesized recently shows an itinerant ferromagnetic character. We investigated this ferromagnetic BaRuO3 using first principles calculations. A few van Hove singularities appear around the Fermi energy, causing unusually high magnetovolume effects of $ΔM/Δa$ ~ 4.3 $μ_B$/Åas well as a Stoner instability [IN(0) ~ 1.2]. At the optimized lattice parameter a, the magnetic moment M is 1.01 $μ_B$ in the local spin de…
A three-step route has been developed for the synthesis of a new oxygen-ordered double perovskite, BaYMn2O5.5 or Ba2Y2Mn4O11. (i) The A-site cation ordered perovskite, BaYMn2O5+d, is first synthesized at d ~ 0 by an oxygen-getter-controlled low-O2-pressure encapsulation technique utilizing FeO as the getter for excess oxygen. (ii) The as-synthesized, oxygen-deficient BaYMn2O5.0 phase is then readily oxygenated to the d ~ 1 level by means of 1-atm-O2 annealing at low temperatures. (iii) By annealing this fully-oxygenated BaYMn2O6.0 in flowing N2 gas at moderate temperatures the new intermediate…
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…
The oxygen-deficient perovskite cobaltite SrCo1-xNbxO3-d was synthesized by direct solid-state reaction and its magnetotransport properties were investigated. This cobaltite exhibits an unusual ferromagnetic behavior with a transition temperature Tm = 130-150 K and a spin glass like behavior below Tm. Importantly, this phase reaches a large magnetoresistance (MR) value, MR = -(rH - r0) / r0 = 30% at 5 K in 7 T. The large MR effect is believed to be related to the disordered magnetic state induced by the Nb-for-Co substitution.
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.
A new 3d-5d hybridized quadruple perovskite oxide, CaCu3Mn2Ir2O12, was synthesized by high-pressure and high-temperature methods. The Rietveld structure analysis reveals that the compound crystallizes in an AA'3B4O12-type perovskite structure with space group Im-3, where the Ca and Cu are 1:3 ordered at fixed atomic positions. At the B site the 3d Mn and the 5d Ir ions are disorderly distributed due to a rare equal +4 charge states for both of them as determined by X-ray absorption spectroscopy. The competing antiferromagnetic and ferromagnetic interactions among Cu2+, Mn4+, and Ir4+ ions give…
We have investigated spin and orbital magnetic moments of the Re 5d ion in the double perovskites A2FeReO6 (A = Ba, Sr, Ca) by X-ray magnetic circular dichroism (XMCD) at the Re L(2,3) edges. In these ferrimagnetic compounds an unusually large negative spin and positive orbital magnetic moment at the Re atoms was detected. The presence of a finite spin magnetic moment in a 'non-magnetic' double perovskite as observed in the double perovskite Sr2ScReO6 proves that Re has also a small, but finite intrinsic magnetic moment. We further show for the examples of Ba and Ca that the usually neglected …
The ordered double perovskites Sr2CrOsO6 and Ca2CrOsO6 have been synthesized and characterized with neutron powder diffraction, electrical transport measurements, and high field magnetization experiments. Sr2CrOsO6 and Ca2CrOsO6 crystallize with R-3 and P21/n space group symmetry, respectively. Both materials are found to be ferrimagnetic insulators with saturation magnetizations near 0.2 μB. Sr2CrOsO6 orders at 660 K, showing non-monotonic magnetization temperature dependence, while Ca2CrOsO6 orders at 490 K and does not show non-monotonic behavior. Evidence for a theoretically predicted cant…
Powder neutron diffraction experiments have been employed to establish the effects of site-selective magnetic dilution in the Sm2MnMnMn4-x Tix O12 A-site columnar ordered quadruple perovskite manganites (x = 1, x = 2 and x = 3). We show that in all three compositions the Mn ions adopt a collinear ferrimagnetic structure below 27 K, 62 K and 34 K, respectively. An unexpected increase in the ordering temperature was observed between the x = 1 and x = 2 samples, which indicates a considerable departure from mean field behaviour. This result is corroborated by large reductions in the theoretical g…
Polycrystalline samples of double perovskites Ba2BOsO6 (B = Sc, Y, In) were synthesized by solid state reactions. They adopt the cubic double perovskite structures (space group, Fm-3m) with ordered B and Os arrangements. Ba2BOsO6 (B = Sc, Y, In) show antiferromagnetic transitions at 93 K, 69 K, and 28 K, respectively. The Weiss-temperatures are -590 K for Ba2ScOsO6, -571 K for Ba2YOsO6, and -155 K for Ba2InOsO6. Sc3+ and Y3+ have the open-shell d0 electronic configuration, while In3+ has the closed-shell d10. This indicates that a d0 B-type cation induces stronger overall magnetic exchange int…
Unusual strain relaxation and Dirac semimetallic behavior in epitaxial antiperovskite nitrides
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；University of Chinese Academy of Sciences（中国科学院大学）；Northwest University（西北大学）；Southern University of Science and Technology（南方科技大学）
ABO3 perovskite multiferroic La0.5Bi0.5Mn0.5Fe0.5O3.09 where the B-site cations is responsible for the magnetic properties and the A-site cation with lone pair electron is responsible for the ferroelectric properties was synthesized at normal conditions. This oxide exhibits a ferromagnetic transition around 240 K with a well defined hysteresis loop, and a significant reversible remnant polarization below 67K similar to ferroelectric behavior. The magnetic interaction is interpreted by the ferromagnetic Fe3+-O-Mn3+ and antiferromagnetic Fe3+(Mn3+)-O-Fe3+(Mn3+) interactions competed each other, …
The first examples of single crystal epitaxial thin films of a high entropy perovskite oxide are synthesized. Pulsed laser deposition is used to grow the configurationally disordered ABO3 perovskite, Ba(Zr0.2Sn0.2Ti0.2Hf0.2Nb0.2)O3, epitaxially on SrTiO3 and MgO substrates. X-ray diffraction and scanning transmission electron microscopy demonstrate that the films are single phase with excellent crystallinity and atomically abrupt interfaces to the underlying substrates. Atomically-resolved electron energy loss spectroscopy mapping shows a uniform and random distribution of all B-site cations. …
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 …
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…
Due of its polymorphism, Mn$_2$FeSbO$_6$ can be synthesized at high pressures and temperatures as a ferrimagnetic ilmenite or an antiferromagnetic perovskite. The structural phase transformation is discussed in detail, and magnetic structures are proposed for both phases. The high-pressure Mn$_2$FeSbO$_6$ polymorph is a rare example of $A_2 B'B"$O$_6$ perovskite with solely Mn cations on the $A$-site. Fe and Sb cations are ordered on the $B$-sites. Theoretical calculations for the perovskite phase suggest a complex magnetic structure, holding an electronic polarization.
Magnetic materials with noncoplanar magnetic structures can show unusual physical properties driven by nontrivial topology. Topologically-active states are often multi-q structures, which are challenging to stabilize in models and to identify in materials. Here, we use inelastic neutron-scattering experiments to show that the insulating double perovskites Ba2YRuO6 and Ba2LuRuO6 host a noncoplanar 3-q structure on the face-centered cubic lattice. Quantitative analysis of our neutron-scattering data reveals that these 3-q states are stabilized by biquadratic interactions. Our study identifies do…
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…
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 magnetic properties of (Ca,Sr)RuO_3 and Sr_2YRuO_6 are studied within the context of band structure based Stoner theory. LSDA calculations without recourse to strong correlation effects yield the correct magnetic behavior and order in all cases. Insulating character of Sr_2YRuO_6 is reproduced. The different magnetic states of SrRuO_3 and CaRuO_3 are shown to be due to the different structural distortions. CaRuO_3 is found to be on the verge of a ferromagnetic instability. O p states hybridize strongly with Ru d states in all three compounds, and O, through this hybridization plays an unus…
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…
Unusual temperature and doping dependence of the Mn 3d spectral functions of manganese perovskites Nd1-xSrxMnO3 has been revealed by the high-resolution Mn 2p-3d resonance photoemission. The temperature-dependent spectra cannot be explained by any theoretical model currently under debate, while showing evidence for a microscopic and dynamic phase segregation. The experimental results strongly suggest that the competition of both the dynamical and static Jahn-Teller effects with ferromagnetic ordering at high and low temperatures, respectively, is responsible for the actual electronic states.
The structural and magnetic properties of double perovskiteTb2CoMnO6 have been investigated. Electronic structure analysis by XPS study reveals the presence of mixed oxidation state (Mn4+/Mn3+ and Co2+/Co3+) of B-site ions. The dc and ac magnetization measurements reveal different interesting phases such as Griffith phase, re-entrant spin glass, metamagnetic steps, Hopkinson like peak and also unusual slow relaxation. The M-H curve indicates the presence of competing AFM/FM interactions. The disorder in Tb2CoMnO6 leads to spin frustration at low temperature giving rise to the re-entrant spin g…
We systematically synthesized perovskite-type oxides Sr1-xCaxCoO3 containing unusually high valence Co4+ ions by a high pressure technique, and investigated the effect of systematic lattice change on the magnetic and electronic properties. As the Ca content x exceeds about 0.6, the structure changes from cubic to orthorhombic, which is supported by the first-principles calculations of enthalpy. Upon the orthorhombic distortion, the ground state remains to be apparently ferromagnetic with a slight drop of the Curie temperature. Importantly, the compounds with x larger than 0.8 show antiferromag…
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…
A metastable perovskite BiFe0.5Sc0.5O3 synthesized under high-pressure (6 GPa) and high- temperature (1500 K) conditions was obtained in two different polymorphs, antipolar Pnma and polar Ima2, through an irreversible behaviour under a heating/cooling thermal cycling. The Ima2 phase represents an original type of a canted ferroelectric structure where Bi3+ cations exhibit both polar and antipolar displacements along the orthogonal [110]p and [1-10]p pseudocubic directions, respectively, and are combined with antiphase octahedral tilting about the polar axis. Both the Pnma and Ima2 structural m…
In the present work, we address the question of an impurity-related origin of the colossal magnetocapacitive effect in the spinel system CdCr2S4. We demonstrate that a strong variation in the dielectric constant below the magnetic transition temperature or in external magnetic fields also arises in crystals prepared without chlorine. This excludes that an inhomogeneous distribution of chlorine impurities at the surface or in the bulk material gives rise to the unusual effects in the spinel multiferroics. In addition, we show that colossal magnetocapacitive effects can be also generated in chlo…
We report the structural transformation of hexagonal Ba3YIr2O9 to a cubic double perovskite form (stable in ambient conditions) under an applied pressure of 8GPa at 1273K. While the ambient pressure (AP) synthesized sample undergoes long-range magnetic ordering at 4K, the high pressure(HP) synthesized sample does not order down to 2K as evidenced from our susceptibility, heat capacity and nuclear magnetic resonance (NMR) measurements. Further, for the HP sample, our heat capacity data have the form gamma*T+beta*T3 in the temperature (T) range of 2-10K with the Sommerfeld coefficient gamma=10mJ…
Compositionally tunable vanadium oxyhydrides Sr2VO4-xHx (x = 0 - 1) without considerable anion vacancy were synthesized by high-pressure solid state reaction. The crystal structures and their properties were characterized by powder neutron diffraction, synchrotron X-ray diffraction, thermal desorption spectroscopy, and first-principles density functional theory (DFT) calculations. The hydrogen anions selectively replaced equatorial oxygen sites in the VO6 layers via statistical substitution of hydrogen in the low x region (x < 0.2). A new orthorhombic phase (Immm) with an almost entirely hydro…
We have studied Ir spin and orbital magnetic moments in the double perovskites La$_{2-x}$Sr$_x$CoIrO$_6$ by x-ray magnetic circular dichroism. In La$_2$CoIrO$_6$, Ir$^{4+}$ couples antiferromagnetically to the weak ferromagnetic moment of the canted Co$^{2+}$ sublattice and shows an unusually large negative total magnetic moment (-0.38\,$μ_{\text B}$/f.u.) combined with strong spin-orbit interaction. In contrast, in Sr$_2$CoIrO$_6$, Ir$^{5+}$ has a paramagnetic moment with almost no orbital contribution. A simple kinetic-energy-driven mechanism including spin-orbit coupling explains why Ir is …
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}…
We synthesize and study single crystals of a new double-perovskite Sr2YIrO6. Despite two strongly unfavorable conditions for magnetic order, namely, pentavalent Ir5+(5d4) ions which are anticipated to have Jeff=0 singlet ground states in the strong spin-orbit coupling (SOC) limit, and geometric frustration in a face centered cubic structure formed by the Ir5+ ions, we observe this iridate to undergo a novel magnetic transition at temperatures below 1.3 K. We provide compelling experimental and theoretical evidence that the origin of magnetism is in an unusual interplay between strong non-cubic…
High purity polycrystalline Na0.5La0.5RuO3 was synthesized by a solid state method, and its properties were studied by magnetic susceptibility, heat capacity and resistivity measurements. We find it to be a tetragonal perovskite, in contrast to an earlier report, with random La/Na mixing. With a Curie-Weiss temperature of -231 K and effective moment of 2.74 uB/mol-Ru, there is no magnetic ordering down to 1.8 K. A broad hump at 1.4 K in the heat capacity, however, indicates the presence of a glassy magnetic transition, which we attribute to the influence of the random distribution of Na and La…
Normally $4d$ or $5d$ transition metals are in a low-spin state. Here using first-principles calculations, we report on a rare case of a high-spin $S$=1 magnetic state for the Ag$^{3+}$ ion in the double perovskite Cs$_{2}$KAgF$_{6}$. We also explored a possibility of a conventional low-spin $S$=0 ground state and find an associated tetragonal distortion to be 0.29 Å. However, the lattice elastic energy cost and the Hund exchange loss exceed the e$_{g}$ crystal-field energy gain, thus making the low-spin tetragonal structure less favorable than the high-spin cubic structure. We conclude that t…
We formulate and study a spin-orbital model for a family of cubic double perovskites with $d^1$ ions occupying a frustrated fcc sublattice. A variational approach and a complimentary analytical analysis reveal a rich variety of phases emerging from the interplay of Hund's and spin-orbit couplings (SOC). The phase digram includes non-collinear ordered states, with or without net moment, and, remarkably, a large window of a non-magnetic disordered spin-orbit dimer phase. The present theory uncovers the physical origin of the unusual amorphous valence bond state experimentally suggested for Ba$_2…
Ruthenates provide comprehensive platform to study a plethora of novel properties, such as quantum magnetism, superconductivity and magnetic fluctuation mediated metal-insulator transition. In this article, we provide an overview of quantum mechanical phenomenology in calcium ruthenium oxide with varying compositions. While the stochiometric composition of CaRuO$_{3}$ exhibits non-Fermi liquid behavior with quasi-criticality, chemically doped compounds depict prominent signatures of quantum magnetic fluctuations at low temperature that in some cases are argued to mediate in metal-insulator tra…
A new layered perovskite-type oxide Ba$_2$RhO$_4$ was synthesized by a high-pressure technique with the support of convex-hull calculations. The crystal and electronic structure were studied by both experimental and computational tools. Structural refinements for powder x-ray diffraction data showed that Ba$_2$RhO$_4$ crystallizes in a K$_2$NiF$_4$-type structure, isostructural to Sr$_2$RuO$_4$ and Ba$_2$IrO$_4$. Magnetic, resistivity, and specific heat measurements for polycrystalline samples of Ba$_2$RhO$_4$ indicate that the system can be characterized as a correlated metal. Despite the clo…
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…
We report an unusual magnetic ground state in single-crystal, double-perovskite Ba2YIrO6 and Sr doped Ba2YIrO6 with Ir5+(5d4) ions. Long-range magnetic order below 1.7 K is confirmed by DC magnetization, AC magnetic susceptibility and heat capacity measurements. The observed magnetic order is extraordinarily delicate and cannot be explained in terms of either a low-spin S=1 state, or a singlet Jeff=0 state imposed by the spin-orbit interactions (SOI). Alternatively, the magnetic ground state appears consistent with a SOI that competes with comparable Hund's rule coupling and inherently large e…
A-site ordered perovskites, CaCu$_3$B$_4$O$_{12}$, which are derivatives of conventional ABO$_3$ perovskites, exhibit varying electronic and magnetic properties. With the objective of examining the role of Cu in this work, we have studied CaCu$_3$Ti$_4$O$_{12}$ and CaCu$_3$Zr$_4$O$_{12}$ and presented the cause of the crystallization of A-site ordered perovskite from conventional ABO$_3$ perovskite and the underlying mechanism leading to the stabilization of non-trivial and experimentally estabilished G-type antiferromagnetic (G-AFM) ordering in these systems. The first-principles electronic s…
Selenium and tellurium are among the few elements that form $AB$O$_3$ perovskite structures with a four valent ion in the $A$ site. This leads to highly distorted structures and unusual magnetic behavior. Here we investigate the Co and Ni selenite and tellurite compounds, CoSeO$_3$, CoTeO$_3$, NiSeO$_3$ and NiTeO$_3$ using first principles calculations. We find an interplay of crystal field and Jahn-Teller distortions that underpin the electronic and magnetic properties. While all compounds are predicted to show an insulating G-type antiferromagnetic ground state, there is a considerable diffe…
Using first-principles density functional theory, we have investigated the electronic and magnetic properties of recently synthesized and characterized 5d double-perovskites Sr2BOsO6 (B=Y, In, Sc). The electronic structure calculations show that in all compounds, the Os5+ (5d3) site is the only magnetically active one, while Y3+, In3+ and Sc3+ remain in nonmagnetic states, with Sc/Y and In featuring d0 and d10 electronic configurations, respectively. Our studies reveal the important role of closed-shell (d10) versus open-shell (d0) electronic configurations of the nonmagnetic sites in determin…
