A procedure is outlined for the determination of magnetic exchange constants in anisotropic perovskite anitferromagnets using powder inelastic neutron scattering. Spin wave densities-of-states are measured using time-of-flight inelastic neutron scattering for LaMnO$_{3}$ ($A$-type antiferromagnet), LaVO$_{3}$ ($C$-type), and LaFeO$_{3}$ ($G$-type) and compared to Heisenberg model calculations. The anisotropy of in-plane ($J_{ab}$) and out-of-plane ($J_{c}$) exchange constants can be obtained from the data. The procedure quickly determines the magnetic exchange interactions without the need for single-crystal dispersion measurements and allows for rapid systematic studies of the evolution of magnetism in perovskite systems.
Magnetism-induced negative thermal expansion (NTE) observed in inverse perovskite antiferromagnets Mn3AN (A=Zn, Ga, etc.) is theoretically studied by a classical spin model with competing bond-length-dependent exchange interactions. We numerically reproduce the crystal-volume expansion upon cooling triggered by a non-coplanar antiferromagnetic order and show that the expansion occurs so as to maximize an energy gain of the nearest-neighbor antiferromagnetic interactions. This mechanism is not specific to inverse perovskite magnets and might also be expected in magnets with other crystal struct…
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.
The magnetic susceptibility, crystal and magnetic structures, and electronic structure of double perovskite Sr2ScOsO6 are reported. Using both neutron and x-ray powder diffraction we find that the crystal structure is monoclinic P21/n from 3.5 to 300 K. Magnetization measurements indicate an antiferromagnetic transition at TN=92K, one of the highest transition temperatures of any double perovskite hosting only one magnetic ion. Type I antiferromagnetic order is determined by neutron powder diffraction, with an Os moment of only 1.6(1) muB, close to half the spin-only value for a crystal field …
We have investigated the structural and magnetic properties of antiferroelectric $A_2$CoTeO$_6$ perovskites with $A$ = Cd, Ca, Sr, Pb, and Ba. All compounds are antiferromagnetic at low temperatures, with the antiferromagnetic transition temperature slightly decreasing with decreasing ionic size of the $A$ cation. Such a decrease in antiferromagnetic interaction is not observed in $A^{2+}_2$Co$M^{6+}$O$_6$ materials with other $M^{6+}$ cations of similar ionic sizes, suggesting that Te$^{6+}$ cations affect the electronic and in turn the magnetic structure of the system.
The layered antiferromagnet FePS$_3$ has been shown to undergo a structural transition under pressure linked to an insulator-metal transition, with two incompatible models previously proposed for the highest-pressure structure. We present a study of the high-pressure crystal structures of FePS$_3$ using both single-crystal and powder x-ray diffraction. We show that the highest pressure transition involves a collapse of the inter-planar spacing of this material, along with an increase in symmetry from a monoclinic to a trigonal structure, to the exclusion of other models. The extent of this vol…
Inelastic neutron scattering experiments show that spin dynamics in the charge ordered insulating ground state of the double-layer perovskite YBaFe2O5 is well described in terms of eg superexchange interactions. Above the Verwey transition at TV = 308 K, t2g double exchange-type conduction within antiferromagnetic FeO2--BaO--FeO2 double layers proceeds by an electron hopping process that requires a spin flip of the five-fold coordinated Fe ions, costing an energy 5<J>S^2 of approximately 0.1 eV. The hopping process disrupts near-neighbor spin correlations, leading to massive damping of zone-bo…
The 5d5 iridate CaIrO3 is isostructural with the post-perovskite phase of MgSiO3, recently shown to occur under extreme pressure in the lower Earth's mantle. It therefore serves as an analogue of post-perovskite MgSiO3 for a wide variety of measurements at ambient conditions or achievable with conventional multianvile pressure modules. By multireference configuration-interaction calculations we here provide essential information on the chemical bonding and magnetic interactions in CaIrO3. We predict a large antiferromagnetic superexchange of 120 meV along the c axis, the same size with the int…
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…
We theoretically investigate magnetic properties of Sr$_2$TcO$_4$, a 4d transition-metal layered perovskite of the K$_2$NiF$_4$-type with half-filled t$_{2g}$ states. The effect of local Coulomb repulsion between the t$_{2g}$ orbitals is included within the density-functional theory (DFT)+U and DFT+dynamical mean-field theory (DMFT) methods. The DFT+DMFT predicts paramagnetic Sr$_2$TcO$_4$ to be close to the Mott insulator-to-metal transition, similarly to the cubic compound SrTcO$_3$. The inter-site exchange interactions computed within the DFT+DMFT framework point to a strong antiferromagnet…
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…
The double perovskite ${\rm La}_2{\rm NiTiO}_6$ is identified as a three-dimensional $S=1$ quantum magnet. By means of Density Functional Theory we demonstrate that this material is a high-spin $d$-electron system deep in the Heisenberg limit and establish that its paramagnetic Mott phase persists down to low temperatures ($T_{\rm N}$=25K) not because of frustration effects but rather for the extreme strong coupling physics. Our many-body calculations on an $ab$ $initio$-derived multi-orbital basis predict indeed a kinetic energy gain when entering the magnetically ordered phase. ${\rm La}_2{\…
Structural, magnetic and electric properties of a metal-ordered perovskite YBaMn2O6 have been studied by means of powder X-ray diffraction, DSC, magnetic susceptibility, and electric resistivity. It is found that this material undergoes a 1st order structural phase transition at Tc1=520 K, from a pseudo orthorhombic (monoclinic) phase to a pseudo tetragonal (monoclinic) one. Accompanied by this transition, the susceptibility exhibits a sharp drop, where ferromagnetic exchange interaction becomes antiferromagnetic. Furthermore, two more transitions, a metal-insulator transition at Tc2=480 K and…
We measured the electrical resistivity, AC magnetic susceptibility, and specific heat of the cubic double perovskite Ba$_2$MgReO$_6$ under pressure. The application of pressure leads to a gradual increase in the transition temperature to the canted antiferromagnetic order, while the quadrupolar order is suppressed above 5 GPa, at which a collinear antiferromagnetic state appears. The obtained unit cell volume-temperature phase diagram for the compound as well as the related compounds suggests that Ba$_2$MgReO$_6$ exists near the phase boundary between the noncollinear and the collinear antifer…
We theoretically study the anomalous Hall effect (AHE) in perovskites with antiferromagnetic (AFM) orderings. By studying the multiorbital Hubbard model for $d$ electrons in perovskite transition metal oxides under the GdFeO$_3$-type distortion within the Hartree-Fock approximation, we investigate the behavior of intrinsic AHE owing to the atomic spin-orbit coupling via the linear response theory. We consider the cases where there exist two ($d^2$) and three ($d^3$) electrons in the $t_{2g}$ orbitals, and show that AFM ordered states can exhibit AHE. In the $d^2$ case, $C$-type AFM states give…
The double perovskite Y_2NiMnO_6 displays ferromagnetic transition at Tc = 81 K. The ferromagnetic order at low temperature is confirmed by the saturation value of magnetization (M_s) and also, validated by the refined ordered magnetic moment values extracted from neutron powder diffraction data at 10 K. This way, the dominant Mn4+ and Ni2+ cationic ordering is confirmed. The cation-ordered P 21/n nuclear structure is revealed by neutron powder diffraction studies at 300 and 10 K. Analysis of frequency dependent dielectric constant and equivalent circuit analysis of impedance data takes into a…
Inverse Melting of 3D Antiferromagnetic Order in Multi-sublattice Magnetic Perovskites
University College London（伦敦大学学院）；STFC Rutherford Appleton Laboratory（STFC卢瑟福阿普顿实验室）；National Institute for Materials Science（材料科学国家研究所）；Hokkaido University（北海道大学）；Osaka University（大阪大学）；Durham University（杜伦大学）
We carried out detailed studies of the magnetic structure, magnetoelastic coupling, and thermal properties of EuCrO$_3$ nano-powders from room temperature to liquid helium temperature. Our neutron powder diffraction and X-ray powder diffraction measurements provide precise atomic positions of all atoms in the cell, especially for the light oxygen atoms. The low-temperature neutron powder diffraction data revealed extra Bragg peaks of magnetic origin which can be attributed to a $G_x$ antiferromagnetic structure with an ordered moment of $\sim$ 2.4 $μ_{\rm B}$ consistent with the $3d^3$ electro…
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 …
The novel electronic state of the canted antiferromagnetic (AFM) insulator, strontium iridate (Sr2IrO4) has been well described by the spin-orbit-entangled isospin Jeff = 1/2, but the role of isospin in transport phenomena remains poorly understood. In this study, antiferromagnet-based spintronic functionality is demonstrated by combining unique characteristics of the isospin state in Sr2IrO4. Based on magnetic and transport measurements, large and highly anisotropic magnetoresistance (AMR) is obtained by manipulating the antiferromagnetic isospin domains. First-principles calculations suggest…
By combining dielectric, specific heat, and magnetization measurements and high-resolution neutron powder diffraction, we have investigated the thermodynamic and magnetic/structural properties of the metastable orthorhombic perovskite ErMnO_3 prepared by high-pressure synthesis. The system becomes antiferromagnetically correlated below 42 K and undergoes a lock-in transition at 28 K with propagation wave vector (0,k_b,0), which remains incommensurate at low temperature. The intercorrelation between the magnetic structure and electric properties and the role of the rare earth moment are discuss…
Exchange bias is usually rationalized invoking spin pinning effects caused by uncompensated antiferromagnetic interfaces. However, for compensated antiferromagnets other extrinsic factors, such as interface roughness or spin canting, have to be considered to produce a small uncompensation. As an alternative, here we propose two (related) possible mechanisms, driven by the intrinsic Dzyaloshinskii-Moriya interaction and ferroelectric polarization, for the explanation of exchange bias effects in perovskites with compensated G-type antiferromagnetism. One of the mechanisms is only active when a m…
We have performed magnetic susceptibility, heat capacity, neutron powder diffraction, and muon spin relaxation experiments to investigate the magnetic ground states of the 5$d^2$ double perovskites Sr$_2$YReO$_6$ and Sr$_2$InReO$_6$. We find that Sr$_2$YReO$_6$ is a spin glass, while Sr$_2$InReO$_6$ hosts a non-magnetic singlet state. By making detailed comparisons with other 5$d^2$ double perovskites, we argue that a delicate interplay between spin-orbit coupling, non-cubic crystal fields, and exchange interactions plays a key role in the great variation of magnetic ground states observed for…
Oxide double perovskites wherein octahedra formed by both 3d elements and sp-based heavy elements give rise to unconventional magnetic ordering and correlated quantum phenomena crucial for futuristic applications. Here, by carrying out experimental and first principles investigations, we present the electronic structure and magnetic phases of Ba2MnTeO6, where Mn^2+ ions with S = 5/2 spins constitute a perfect triangular lattice. The magnetic susceptibility reveals a large Curie- Weiss temperature -152 K suggesting the presence of strong antiferromagnetic interactions between Mn^2+ moments in t…
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 present a neutron powder diffraction study of the monoclinic double perovskite systems Nd2NaB'O6 (B' = Ru, Os), with magnetic atoms occupying both the A and B' sites. Our measurements reveal coupled spin ordering between the Nd and B' atoms with magnetic transition temperatures of 14 K for Nd2NaRuO6 and 16 K for Nd2NaOsO6. There is a Type I antiferromagnetic structure associated with the Ru and Os sublattices, with the ferromagnetic planes stacked along the c-axis and [110] direction respectively, while the Nd sublattices exhibit complex, canted antiferromagnetism with different spin arrang…
Nontrivial magnetic orders in the inverse-perovskite manganese nitrides are theoretically studied by constructing a classical spin model describing the magnetic anisotropy and frustrated exchange interactions inherent in specific crystal and electronic structures of these materials. With a replica-exchange Monte-Carlo technique, a theoretical analysis of this model reproduces the experimentally observed triangular Γ^{5g} and Γ^{4g} spin ordered patterns and the systematic evolution of magnetic orders. Our work solves a 40-year-old problem of nontrivial magnetism for the inverse-perovskite mang…
Theoretical DFT calculations using GGA+U and HSE06 frameworks enabled vibrational mode assignment and partial (atomic) phonon DOS determination in KAgF3 perovskite, a low-dimensional magnetic fluoroargentate(II). Twelve bands in the spectra of KAgF3 were assigned to either IR active or Raman active modes, reaching very good correlation with experimental values (R2>0.997). Low-temperature Raman measurements indicate that the intriguing spin-Peierls-like phase transition at 230 K is an order-disorder transition and it does not strongly impact the vibrational structure of the material.
The magnetic structure of Ca$_2$MnReO$_6$ double perovskite is investigated by neutron powder diffraction and bulk magnetization, showing dominant non-collinear Mn magnetic moments [$4.35(7)$ $μ_B$] that are orthogonally aligned with the small Re moments [$0.22(4)$ $μ_B$]. $Ab$-initio electronic structure calculations show that the strong spin-orbit coupling for Re $5d$ electrons combined with a relatively modest on-site Coulomb repulsion ($U_{eff}^{Re} \gtrsim 0.6$ eV) is sufficient to render this material insulating. This is a rare example of spin-orbit assisted Mott insulator outside the re…
The usual classical behaviour of S = 3/2, B-site ordered double perovskites generally results in simple, commensurate magnetic ground states. In contrast, heat capacity and neutron powder diffraction measurements for the S = 3/2 systems La2NaB'O6 (B' = Ru, Os) reveal an incommensurate magnetic ground state for La2NaRuO6 and a drastically suppressed ordered moment for La2NaOsO6. This behaviour is attributed to the large monoclinic structural distortions of these double perovskites. The distortions have the effect of weakening the nearest neighbour superexchange interactions, presumably to an en…
Topotactic transformations between related crystal structures are a powerful emerging route for the synthesis of novel quantum materials. Whereas most such "soft chemistry" experiments have been carried out on polycrystalline powders or thin films, the topotactic modification of single crystals -- the gold standard for physical property measurements on quantum materials -- has proven remarkably difficult. Here, we report the topotactic reduction of La$_{1-x}$Ca$_{x}$NiO$_3$ single-crystals to La$_{1-x}$Ca$_{x}$NiO$_{2+δ}$ using CaH$_2$ as the reducing agent. The transformation from the three-d…
The Fe electronic structure and magnetism in (i) monoclinic Ca$_2$FeReO$_6$ with a metal-insulator transition at $T_{MI} \sim 140$ K and (ii) quasi-cubic half-metallic Ba$_2$FeReO$_6$ ceramic double perovskites are probed by soft x-ray absorption spectroscopy (XAS) and magnetic circular dichroism (XMCD). These materials show distinct Fe $L_{2,3}$ XAS and XMCD spectra, which are primarily associated with their different average Fe oxidation states (close to Fe$^{3+}$ for Ca$_2$FeReO$_6$ and intermediate between Fe$^{2+}$ and Fe$^{3+}$ for Ba$_2$FeReO$_6$) despite being related by an isoelectron…
We theoretically show that materials with perovskite-type crystal structures provide a platform for spin current generation, taking advantage of a mechanism requiring neither the spin-orbit coupling nor a ferromagnetic moment, but is based on spin-split band structures in certain kinds of collinear antiferromagnetic states. By investigating a multiband Hubbard model for transition metal compounds by means of the Hartree-Fock approximation and the Boltzmann transport theory, we find that a pure spin current is induced by an electric field applied to a C-type antiferromagnetic metallic phase. Th…
We present a combined neutron and synchrotron powder diffraction study of the crystal and magnetic structure of VOCl. The occurrence of antiferromagnetic order in VOCl is accompanied by a monoclinic distortion. The high sensitivity of the magnetic interaction parameters on V-O-V bond angles and V-V distances yields strong magnetoelastic coupling which implies the structural distortion below T$_N$ as well as anomalous structural effects in the paramagnetic phase.
We report structural, magnetic and dielectric properties of layered perovskite materials LnBaCuFeO5 (Ln = La and Lu). LaBaCuFeO5 shows magnetic cluster glass behavior below 60 K owing to the competing ferromagnetic and antiferromagnetic exchange interactions. Glassy dynamics of electric dipoles has also been observed in the vicinity of the magnetic glass transition temperature. The presence of significant coupling between spin and polar degrees of freedom results in the multiglass feature in LaBaCuFeO5. The LuBaCuFeO5 compound undergoes YBaCuFeO5 like commensurate to incommensurate antiferroma…
Double perovskite iridates $A_2$ZnIrO$_6$ ($A$ = alkaline or lanthanide) show complex magnetic behaviors ranging from weak ferromagnetism to successive antiferromagnetic transitions. Here we report the static ($dc$) and dynamic ($ac$) magnetic susceptibility, and neutron powder diffraction measurements for $A$ = La and Nd compounds to elucidate the magnetic ground state. Below 10~K, the $A$ = La compound is best described as canted iridium moments in an antiferromagnet arrangement with a propagation vector \textbf{k} = 0 and a net ferromagnetic component along the $c$-axis. On the other hand, …
The rare-earth perovskite TbScO$_3$ has been widely used as a substrate for the growth of epitaxial ferroelectric and multiferroic thin films, while its detailed low-temperature magnetic properties were rarely reported. In this paper, we performed detailed magnetization, specific heat and single crystal neutron scattering measurements, along with the crystalline electric field calculations to study the low-temperature magnetic properties of TbScO$_3$. All our results suggest the magnetic Tb$^{3+}$ has an Ising-like pseudo-doublet ground state at low temperatures. Due to the constrain of local …
We report an experimental investigation of the two-dimensional ${J}_{\rm eff}$ = 1/2 antiferromagnetic Mott insulator by varying the interlayer exchange coupling in [(SrIrO$_3$)$_1$, (SrTiO$_3$)$_m$] ($m$ = 1, 2 and 3) superlattices. Although all samples exhibited an insulating ground state with long-range magnetic order, temperature-dependent resistivity measurements showed a stronger insulating behavior in the $m$ = 2 and $m$ = 3 samples than the $m$ = 1 sample which displayed a clear kink at the magnetic transition. This difference indicates that the blocking effect of the excessive SrTiO$_…
We present the magnetic structure of $\mathrm{TmMn_3O_6}$, solved via neutron powder diffraction - the first such study of any $R\mathrm{Mn_3O_6}$ A-site columnar-ordered quadruple perovskite to be reported. We demonstrate that long range magnetic order develops below 74 K, and at 28 K a spin-flop transition occurs driven by $f$-$d$ exchange and rare earth single ion anisotropy. In both magnetic phases the magnetic structure may be described as a collinear ferrimagnet, contrary to conventional theories of magnetic order in the manganite perovskites. Instead, we show that these magnetic structu…
The double-perovskite A$_2$BB'O$_6$ with heavy transition metal ions on the ordered B' sites is an important family of compounds to study the interplay between electron correlation and spin-orbit coupling (SOC). Here we prepared high-quality Sr$_2$MgReO$_6$ powder and single-crystal samples and performed non-resonant and resonant synchrotron x-ray diffraction experiments to investigate its magnetic ground state. By combining the magnetic susceptibility and heat capacity measurements, we conclude that Sr$_2$MgReO$_6$ exhibits a layered antiferromagnetic (AF) order at temperatures below $\sim$ 5…
The incommensurate magnetic response of the normal-state cuprate perovskites is interpreted based on Mori's memory function approach and the t-J model of Cu-O planes. In agreement with experiment the calculated dispersion of the susceptibility maxima has the shape of two parabolas with upward and downward branches which converge at the antiferromagnetic wave vector. The maxima are located at $({1/2},{1/2}\pmδ)$, $({1/2}\pmδ,{1/2})$ and at $({1/2}\pmδ,{1/2}\pmδ)$, $({1/2}\pmδ,{1/2}\mpδ)$ in the lower and upper parabolas, respectively. The upper parabola reflects the dispersion of magnetic excit…
In this work, we report on the synthesis and magnetic properties of a series of double perovskites Ln$_2$ZnIrO$_6$ with Ln = Nd, Sm, Eu & Gd. These compounds present new examples of the rare case of double perovskites (general formula A$_2$BB'O$_6$) with a magnetic 4f -ion on the A-site in combination with the strongly spin-orbit coupled 5d-transition metal ion Ir$^{4+}$ on the B-sublattice. We discuss the impact of different rare earths on the macroscopic magnetic properties. Gd$_2$ZnIrO$_6$ and Eu$_2$ZnIrO$_6$ show weak canted antiferromagnetic order below T$_N$ = 23 K and T$_N$ = 12 K, resp…
We investigate the metal-insulator transition in the layered Ruddelsden Popper series of strontium iridates Srn+1IrnO3n+1. Tight-binding models of t2g orbitals for n = 1, 2, and infinity are constructed, and changes in band dispersion due to dimensionality and spin-orbit coupling are presented. Identifying the states near the Fermi level to be predominantly Jeff = 1/2, we use an effective Hubbard model to study the effect of correlations. Transitions from a metallic state to various magnetically ordered states at different critical interactions are obtained. A canted antiferromagnetic insulato…
We report the structural, magnetic and thermodynamic properties of the double perovskite compound La2CuIrO6 from X-ray, neutron diffraction, neutron depolarization, dc magnetization, ac susceptibility, specific heat, muon-spin-relaxation (uSR), electron-spin-resonance (ESR) and nuclear magnetic resonance (NMR) measurements. Below ~113 K, short-range spin-spin correlations occur within the Cu2+ sublattice. With decreasing temperature, the Ir4+ sublattice progressively involves in the correlation process. Below T = 74 K, the magnetic sublattices of Cu (spin s = 1/2) and Ir (pseudospin j = 1/2) i…
Raman spectroscopic signature of Kitaev magnetism and complex spin-lattice coupling in S = 1/2 antiferromagnet SrLaCoNbO$_6$ double perovskite
Ames National Laboratory, U.S. Department of Energy, Iowa State University（艾姆斯国家实验室）；Department of Physics, Indian Institute of Technology Delhi（德里印度理工学院物理系）；School of Physics, The University of New South Wales (UNSW)（新南威尔士大学物理学院）
We investigated the crystal and magnetic structures of the spin-1/2 frustrated antiferromagnet Cu3Mo2O9 in which the spin system consists of antiferromagnetic chains and dimers. The space group at room temperature has been reported to be orthorhombic Pnma (No. 62). We infer that the space group above TN = 7.9 K is monoclinic P2_1/m (No. 11) from the observation of reflections forbidden in Pnma in x-ray powder diffraction experiments at room temperature. We determined the magnetic structure of Cu3Mo2O9 in neutron powder diffraction experiments. Magnetic moments on dimer sites lie in the ac plan…
Unveiling the magnetic ground states in the iridate double perovskite Pr(2-x)SrxMgIrO6 (x = 0 and 0.5) series
ISIS Neutron and Muon Source, STFC, Rutherford Appleton Laboratory（STFC 卢瑟福·阿普尔顿实验室 ISIS 中子与μ子源）；School of Materials Science, Indian Association for the Cultivation of Science（印度科学促进协会材料科学学院）；Institut Laue-Langevin（朗之万研究所）；University of Johannesburg（约翰内斯堡大学）
KCrF3 represents another prototypical orbital-ordered perovskite, where Cr2+ possesses the same electronic configuration of 3d4 as that of strongly Jahn-Teller distorted Mn3+ in many CMR manganites. The crystal and magnetic structures of KCrF3 compound are investigated by using polarized and unpolarized neutron powder diffraction methods. The results show that the KCrF3 compound crystallizes in tetragonal structure at room temperature and undergoes a monoclinic distortion with the decrease in temperature. The distortion of the crystal structure indicates the presence of cooperative Jahn-Teller…
We consider strongly spin-orbit coupled double perovskites A$_2$BB'O$_6$ with B' magnetic ions in either $d^1$ or $d^2$ electronic configuration and non-magnetic B ions. We provide insights into several experimental puzzles, such as the predominance of ferromagnetism in $d^1$ versus antiferromagnetism in $d^2$ systems, the appearance of negative Curie-Weiss temperatures for ferromagnetic materials, and the size of effective magnetic moments. We develop and solve a microscopic model with both spin and orbital degrees of freedom within the Mott insulating regime at finite temperature using mean …
The B-site ordered double perovskite Ba2CaOsO6 was studied by d.c. magnetic susceptibility, powder neutron diffraction and muon spin relaxation methods. The lattice parameter is a = 8.3619(6) A at 280K and cubic symmetry (Fm-3m) is retained to 3.5K with a = 8.3426(5) A. Curie-Weiss susceptibility behavior is observed for T > 100K and the derived constants are C = 0.3361(1)emu-K/mole and T_CW = -156.2(3) K, in excellent agreement with literature values. This Curie constant is much smaller than the spin-only value of 1.00 emu-K/mole for a 5d^2 Os6+ configuration, indicating a major influence of …
5d iridates have shown vast emergent phenomena due to a strong interplay among its lattice, charge and spin degrees of freedom, because of which the potential in spintronic application of the thin-film form is highly leveraged. Here we have epitaxially stabilized perovskite SrIr$_{0.8}$Sn$_{0.2}$O$_3$ on [001] SrTiO$_3$ substrates through pulsed laser deposition and systematically characterized the structural, electronic and magnetic properties. Physical properties measurements unravel an insulating ground state with a weak ferromagnetism in the compressively strained epitaxial film. The octah…
We report the understanding of the electronic band structure of $Cs_4CuSb_2Cl_{12}$ perovskite through first-principles density-functional theory calculations. We find that the most stable state has the antiferromagnetic configuration where each $[CuCl_6]$ octahedral chain along the [010] direction is antiferromagnetic. The reasonable band structure of the compound can be obtained only if both the correct magnetic order and the improved exchange interaction of the Cu $\it{d}$ electrons are taken into account.
The magnetic ground state in highly ordered double perovskites LaSr$_{1-x}$Ca$_x$NiReO$_6$ ($x$ = 0.0, 0.5, 1.0) were studied in view of the Goodenough-Kanamori rules of superexchange interactions. In LaSrNiReO$_6$, Ni and Re sublattices are found to exhibit curious magnetic states, but do not show any long range magnetic ordering. The magnetic transition at $\sim$ 255 K is identified with the Re sublattic magnetic ordering. The sublattice interactions are tuned by modifying the Ni-O-Re bond angles via changing the lattice structure through Ca doping. Upon Ca doping, the Ni and Re sublattices …
We report the magnetic properties of $A$-site spinel compound MnSc$_2$Se$_4$. The macroscopic magnetic measurements uncovers successive magnetic transitions at $T_{\rm{N1}}$= 2.04 K, followed by two further transitions at $T_{\rm{N2}}$=1.8 K and $T_{\rm{N3}}$=1.6 K. Neutron powder diffraction reveals that both, $T_{\rm{N2}} < T < T_{\rm{N1}}$ and $T <T_{\rm{N3}}$, orders are associated with the propagation vector $k$=(3/4 3/4 0), while the magnetic structures are collinear amplitude modulated and helical, respectively. Using neutron powder spectroscopy we demonstrated the effect of substitutio…
In their ideal structure, double perovskites like Sr_2FeMoO_6 have alternating Fe and Mo along each cubic axes, and a homogeneous ferromagnetic metallic ground state. Imperfect annealing leads to the formation of structural domains. The moments on mislocated Fe atoms that adjoin each other across the domain boundary have an antiferromagnetic coupling between them. This leads to a peculiar magnetic state, with ferromagnetic domains coupled antiferromagnetically. At short distance the system exhibits ferromagnetic correlation while at large lengthscales the net moment is strongly suppressed due …
A quantum spin liquid state has long been predicted to arise in spin-1/2 Heisenberg square-lattice antiferromagnets at the boundary region between Néel (nearest-neighbor interaction dominates) and columnar (next-nearest-neighbor dominates) antiferromagnetic order. However, there are no known compounds in this region. Here we use $d^{10}$-$d^0$ cation mixing to tune the magnetic interactions on the square lattice while simultaneously introducing disorder. We find spin-liquid-like behavior in the double perovskite Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$, where the isostructural end phases Sr$_2$CuTeO…
