Spin-orbit coupling (SOC) plays a crucial role in magnetic and electronic properties of 5$d$ iridates. In this paper we have experimentally investigated the structural and physical properties of a series of Ir-based double perovskite compounds Pr$_{2-x}$Sr$_x$MgIrO$_6$ ($x$ = 0, 0.5, 1; hereafter abbreviated as PMIO, PSMIO1505, and PSMIO). Interestingly, these compounds have recently been proposed to undergo a transition from the spin-orbit-coupled Mott insulating phase at $x$ = 0 to the elusive half-metallic antiferromagnetic (HMAFM) state with Sr doping at $x$ = 1. However, our detailed magnetic and electrical measurements refute any kind of HMAFM possibility in either of the doped samples. In addition, we establish that within these Pr$_{2-x}$Sr$_x$MgIrO$_6$ double perovskites, changes in Ir-oxidation states (4+ for PMIO to 5+ for PSMIO via mixed 4+/5+ for PSMIO1505) lead to markedly different magnetic behaviors. While SOC on Ir is at the root of the observed insulating behaviors for all three samples, the correlated magnetic properties of these three compounds develop entirely due to the contribution from local Ir moments. Additionally, the magnetic Pr$^{3+}$ (4$f^2$) ions, instead of showing any kind of ordering, only contribute to the total paramagnetic moment. It is seen that the PrSrMgIrO$_6$ sample does not order down to 2 K despite antiferromagnetic interactions. But, the $d^5$ iridate Pr$_2$MgIrO$_6$ shows a sharp antiferromagnetic (AFM) transition at around 14 K, and in the mixed valent Pr$_{1.5}$Sr$_{0.5}$MgIrO$_6$ sample the AFM transition is shifted to a much lower temperature ($\sim$ 6 K) due to weakening of the AFM exchange.
We have successfully synthesized the novel antiferromagnets with Ir$^{4+}$ honeycomb lattice ZnIrO$_3$ and MgIrO$_3$ and investigated their magnetic and thermodynamic properties. The two iridates are isomorphic but exhibit qualitatively different magnetic properties. ZnIrO$_3$ shows antiferromagnetic ordering below 46.6 K, whereas MgIrO$_3$ displays weak ferromagnetic behavior below 31.8 K owing to formation of a canted antiferromagnetic ordering. The measurement of magnetic susceptibility with using an oriented powder sample revealed the presence of an XY-like magnetic anisotropy and a tiltin…
We investigated the magnetic properties of the ilmenite-type iridate CdIrO$_3$ with a honeycomb lattice formed by Ir$^{4+}$ ions prepared via a solid-state metathesis. The magnetization measurements with using the powder sample reveal a large effective magnetic moment and a fairly strong antiferromagnetic interaction, indicating a deviation from the Kitaev model. Considering the relationship between magnetism and crystal structure in CdIrO$_3$ with comparing with the other ilmenite-type iridates ZnIrO$_3$ and MgIrO$_3$, we conclude that insulating CdIrO$_3$ cannot be describe as a $J_{\rm eff}…
We report on an angle resolved photoemission (ARPES) study of bulk electron-doped perovskite iridate, (Sr1-xLax)3Ir2O7. Fermi surface pockets are observed with a total electron count in keeping with that expected from La substitution. Depending on the energy and polarization of the incident photons, these pockets show up in the form of disconnected "Fermi arcs", reminiscent of those reported recently in surface electron-doped Sr2IrO4. Our observed spectral variation is consistent with the coexistence of an electronic supermodulation with structural distortion in the system.
We present genuine bulk Ir 5d jeff states of layered perovskite iridates obtained by hard-x-ray photoemission spectroscopy (HAXPES) with s- and p-polarized lights. HAXPES spectra of Sr2IrO4 and Ba2IrO4 are well reproduced by the quasi-particle densities of states calculated by the local density approximation with dynamical mean-field theory (LDA+DMFT). It is demonstrated that the insulating nature of the iridates is triggered by antiferromagnetic correlation (Slater type) combined with electron correlation (Mott type). The extremely-low-energy bulk-sensitive photoemission spectroscopy reveals …
A theoretical investigation of a plausible construct for electronic structure in iridate perovskites demonstrates the existence of magnetic multipoles hitherto not identified. The strange multipoles, which are parity-even, time-odd and even rank tensors, are absent from the so-called jeff = 1/2 model. We prove that the strange multipoles contribute to magnetic neutron diffraction, and we estimate their contribution to intensities of Bragg spots for Sr2IrO4. The construct encompasses the jeff = 1/2 model, and it is consistent with the known magnetic structure, ordered magnetic moment, and publi…
We have performed inelastic neutron scattering experiments to investigate the magnetic excitations in the quasi-face-centered-cubic (fcc) iridate double perovskites La2ZnIrO6 and La2MgIrO6, which are characterized by A-type antiferromagnetic ground states. The neutron scattering data, which reveal gapped spin wave excitations with a very weak dispersion, are shown to be well-described by theoretical calculations on a model Hamiltonian with dominant Kitaev interactions. Our surprising finding shows that in contrast to honeycomb materials, where the Kitaev interaction manifests itself via comple…
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…
The orthorhombic perovskite SrIrO3 is a semimetal, an intriguing exception in iridates where the strong spin-orbit interaction coupled with electron correlations tends to impose a novel insulating state. We report results of our investigation of bulk single-crystal Sr0.94Ir0.78O2.68 or Ir-deficient, orthorhombic perovskite SrIrO3. It retains the same crystal structure as stoichiometric SrIrO3 but exhibits a sharp, simultaneous antiferromagnetic (AFM) and metal-insulator (MI) transition at 185 K. Above it, the basal-plane resistivity features an extended regime of almost linear-temperature depe…
Iridates with the 5$d^4$ electronic configuration have attracted recent interest due to reports of magnetically-ordered ground states despite longstanding expectations that their strong spin-orbit coupling would generate a $J = 0$ electronic ground state for each Ir$^{5+}$ ion. The major focus of prior research has been on the double perovskite iridates Ba$_2$YIrO$_6$ and Sr$_2$YIrO$_6$, where the nature of the ground states (i.e. ordered vs non-magnetic) is still controversial. Here we present neutron powder diffraction, high energy resolution fluorescence detected x-ray absorption spectrosco…
We report angle-resolved photoemission (ARPES) measurements, density functional and model tight-binding calculations on Ba$_2$IrO$_4$ (Ba-214), an antiferromagnetic ($T_N=230$ K) insulator. Ba-214 does not exhibit the rotational distortion of the IrO$_6$ octahedra that is present in its sister compound Sr$_2$IrO$_4$ (Sr-214), and is therefore an attractive reference material to study the electronic structure of layered iridates. We find that the band structures of Ba-214 and Sr-214 are qualitatively similar, hinting at the predominant role of the spin-orbit interaction in these materials. Temp…
We studied Sr2IrO4 and Sr3Ir2O7 using angle-resolved photoemission spectroscopy (ARPES), making direct experimental determinations of intra- and inter-cell coupling parameters as well as Mott correlations and gap sizes. The results are generally consistent with LDA+U+Spin-orbit coupling (SOC) calculations, though the calculations missed the momentum positions of the dominant electronic states and neglected the importance of inter-cell coupling on the size of the Mott gap. The calculations also ignore the correlation-induced spectral peak widths, which are critical for making a connection to ac…
Transition metal oxides, in particular, 3d or 4d perovskites have provided diverse emergent physics that originates from the coupling of various degrees of freedom such as spin, lattice, charge, orbital, and also disorder. 5d perovskites form a distinct class because they have strong spin-orbit coupling that introduces to the system an additional energy scale that is comparable to bandwidth and Coulomb correlation. Consequent new physics includes novel Jeff = 1/2 Mott insulators, metal-insulator transitions, spin liquids, and topological insulators. After highlighting some of the phenomena app…
Investigation of elementary excitations has advanced our understanding of many-body physics governing most physical properties of matter. Recently spin-orbit excitons have drawn much attention, whose condensates near phase transitions exhibit Higgs mode oscillations, a long-sought physical phenomenon [Nat. Phys. {\bf 13}, 633 (2017)]. These critical transition points resulting from competing spin-orbit coupling (SOC), local crystalline symmetry and exchange interactions, are not obvious in Iridium based materials, where SOC prevails in general. Here, we present results of resonant inelastic x-…
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…
Spin-orbit effects in heavy 5$d$ transition metal oxides, in particular, iridates, have received enormous current interest due to the prediction as well as the realization of a plethora of exotic and unconventional magnetic properties. While a bulk of these works are based on tetravalent iridates ($d^5$), where the counter-intuitive insulating state of the rather extended 5$d$ orbitals are explained by invoking strong spin-orbit coupling, the recent quest in iridate research has shifted to the other valencies of Ir, of which pentavalent iridates constitute a notable representative. In contrast…
We perform a comparative magnetic study on two series of rare-earth (RE) based double perovskite iridates RE2BIrO6 (RE=Pr,Nd,Sm-Gd;B=Zn,Mg), which show Mott insulating state with tunable charge energy gap from ~330 meV to ~560 meV by changing RE cations. For nonmagnetic RE=Eu cations, Eu2MgIrO6 shows antiferromagnetic (AFM) order and field-induced spin-flop transitions below Néel temperature (TN) in comparison with the ferromagnetic (FM)-like behaviors of Eu2ZnIrO6 at low temperatures. For magnetic-moment-containing RE ions, Gd2BIrO6 show contrasting magnetic behaviors with FM-like transition …
The resonant X-ray scattering (magnetic elastic, RXMS, and inelastic, RIXS) of Ir$^{4+}$ at the L$_{2,3}$ edges relevant to spin-orbit Mott insulators A$_{n+1}$Ir$_{n}$O$_{3n+1}$ (A=Sr, Ba, etc.) are calculated using a single-ion model which treats the spin-orbit and tetragonal crystal-field terms on an equal footing. Both RXMS and RIXS in the spin-flip channel are found to display a non-trivial dependence on the direction of the magnetic moment, $\boldsymbolμ$. Crucially, we show that for $\boldsymbolμ$ in the \emph{ab}-plane, RXMS at the L$_2$ edge is zero \emph{irrespective} of the tetragon…
The spin-orbit coupled double perovskite iridate Ba$_2$YIrO$_6$ with $d^4$ occupancy of Ir is considered as a candidate material for a non-magnetic $J=0$ ground state. The issue of existence of such a state in Ba$_2$YIrO$_6$ however has opened up intense debates both in experimental and theoretical studies. In this study, we revisit the issue using \textit{ab-initio} density functional combined with dynamical mean-field theory to investigate the magnetic properties of Ba$_2$YIrO$_6$ down to zero temperature. To reach the ground state, a recently developed impurity solver based on tensor-produc…
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…
Resonant inelastic X-ray scattering (RIXS) experiments performed at the oxygen-$K$ edge on the iridate perovskites {\SIOS} and {\SION} reveal a sequence of well-defined dispersive modes over the energy range up to $\sim 0.8$ eV. The momentum dependence of these modes and their variation with the experimental geometry allows us to assign each of them to specific collective magnetic and/or electronic excitation processes, including single and bi-magnons, and spin-orbit and electron-hole excitons. We thus demonstrated that dispersive magnetic and electronic excitations are observable at the O-$K$…
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…
Quantum magnets with significant bond-directional Ising interactions, so-called Kitaev materials, have attracted tremendous attention recently in the search for exotic spin liquid states. Here we present a comprehensive set of measurements that enables us to investigate the crystal structures, Ir$^{4+}$ single ion properties, and magnetic ground states of the double perovskite iridates La$_2B$IrO$_6$ ($B$ $=$ Mg, Zn) and $A_2$CeIrO$_6$ ($A$ $=$ Ba, Sr) with a large nearest neighbor distance $>$ 5 Angstroms between Ir$^{4+}$ ions. Our neutron powder diffraction data on Ba$_2$CeIrO$_6$ can be re…
The perovskite SrIrO3 is an exotic narrow-band metal owing to a confluence of the strengths of the spin-orbit coupling (SOC) and the electron-electron correlations. It has been proposed that topological and magnetic insulating phases can be achieved by tuning the SOC, Hubbard interactions, and/or lattice symmetry. Here, we report that the substitution of nonmagnetic, isovalent Sn4+ for Ir4+ in the SrIr1-xSnxO3 perovskites synthesized under high pressure leads to a metal-insulator transition to an antiferromagnetic (AF) phase at TN > 225 K. The continuous change of the cell volume as detected b…
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）
We have investigated the electronic structure of iridates in the double perovskite crystal structure containing either Ir$^{4+}$ or Ir$^{5+}$ using hard x-ray photoelectron spectroscopy. The experimental valence band spectra can be well reproduced using tight binding calculations including only the Ir $5d$, O $2p$ and O $2s$ orbitals with parameters based on the downfolding of the density-functional band structure results. We found that regardless of the A and B cations, the A$_2$BIrO$_6$ iridates have essentially zero O $2p$ to Ir $5d$ charge transfer energies. Hence, double perovskite iridat…
The anomalous thermal expansion in a layered 3$d$-5$d$ based triple perovskite iridate Ba$_{3}$CoIr$_{2}$O$_{9}$ is investigated using high resolution synchrotron diffraction. Below the magneto-structural transition at 107\,K, the onset of antiferromagnetic order is associated with a monoclinic distortion of the hexagonal structure. Deeper within the magnetically ordered state, a part of the monoclinic phase distorts even further, and both these structural phases co-exist down to the lowest measured temperatures. We observe negative thermal expansion in this phase co-existence regime, which ap…
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…
By performing resonant inelastic x-ray scattering (RIXS) measurements at the Ir $\mathit{L_{\mathrm{3}}}$ edge, we have investigated the low-energy elementary excitations in a series of double perovskite iridate single crystals, La$_{2}$$\mathit{M}$IrO$_{6}$ ($\mathit{M}$ = Co, Ni, and Zn). Almost dispersionless magnetic excitations at $\sim$ 42(6) meV and $\sim$ 35(5) meV have been observed in crystals containing magnetic 3$\mathit{d}$ ions, La$_{2}$CoIrO$_{6}$ and La$_{2}$NiIrO$_{6}$, respectively. In contrast, this low-energy magnetic excitation is absent in La$_{2}$ZnIrO$_{6}$ in which the…
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$_…
There have been increasing efforts in realizing topological metallic phases with nontrivial surface states. It was suggested that orthorhombic perovskite iridates are classified as a topological crystalline metal (TCM) with flat surface states protected by lattice symmetries. Here we perform first-principles electronic structure calculations for epitaxially stabilized orthorhombic perovskite iridates. Remarkably, two different types of topological surface states are found depending on surface directions. On side surfaces, flat surface states protected by lattice symmetries emerge, manifesting …
5d iridates have shown vast emergent phenomena due to a strong interplay among its lattice, charge and spin degrees of freedom, because of which the potential in spintronic application of the thin-film form is highly leveraged. Here we have epitaxially stabilized perovskite SrIr$_{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…
A three-orbital-model approach for studying spin wave excitations in the strongly spin-orbit coupled layered perovskite iridates is presented which provides a unified description of magnetic excitations as well as the electronic band structure. The calculated spin wave dispersions with realistic three-band parameters are in excellent agreement with the RIXS data for iridates, including the strong AF zone boundary dispersion in the single-layer compound $\rm Sr_2 Ir O_4$ and the large anisotropy gap in the bilayer compound $\rm Sr_3 Ir_2 O_7$. The RIXS spin wave data is shown to provide evidenc…
$J_{eff}$ states in a quasi one dimensional antiferromagnetic spin chain hexagonal Iridates Sr$_3$MIrO$_6$ (M=Mg, Zn, Cd): an $ab-initio$ comparative perspective
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 …
Motivated by the experiments on the rare-earth double perovskites, we propose a generalized Kitaev-Heisenberg model to describe the generic interaction between the spin-orbit-entangled Kramers' doublets of the rare-earth moments. We carry out a systematic analysis of the mean-field phase diagram of this new model. In the phase diagram, there exist large regions with a continuous U(1) or O(3) degeneracy. Since no symmetry of the model protects such a continuous degeneracy, we predict that the quantum fluctuation lifts the continuous degeneracy and favors various magnetic orders in the phase dia…
We investigate magnetic excitations in iridium insulators with pentavalent Ir$^{5+}$ ($5d^4$) ions with strong spin-orbit coupling. We obtain a microscopic model based on the local Ir$^{5+}$ multiplets involving $J=0$ (singlet), $J=1$ (triplet), and $J=2$ (quintet) spin-orbital states. We get effective interactions between these multiplets on square and face-centered-cubic (fcc) structures of magnetic ions in the layered-perovskites and the double-perovkites, in particular Ba$_2$YIrO$_6$. Further, we derive an effective spin-orbital Hamiltonian in terms of bond bosons and explore possible inst…
We report a comprehensive investigation of Ln2NiIrO6 (Ln = La, Pr, Nd) using thermodynamic and transport properties, neutron powder diffraction, resonant inelastic x-ray scattering, and density functional theory (DFT) calculations to investigate the role of A-site cations on the magnetic interactions in this family of hybrid 3d-5d-4f compositions. Magnetic structure determination using neutron diffraction reveals antiferromagnetism for La2NiIrO6, a collinear ferrimagnetic Ni/Ir state that is driven to long range antiferromagnetism upon the onset of Nd ordering in Nd2NiIrO6, and a non-collinear…
The magnetic structure and electronic groundstate of the layered perovskite Ba2IrO4 have been investigated using x-ray resonant magnetic scattering (XRMS). Our results are compared with those for Sr2IrO4, for which we provide supplementary data on its magnetic structure. We find that the dominant, long-range antiferromagnetic order is remarkably similar in the two compounds, and that the electronic groundstate in Ba2IrO4, deduced from an investigation of the XRMS $L_3/L_2$ intensity ratio, is consistent with a $J_{eff}=1/2$ description. The robustness of these two key electronic properties to …
The synthesis and characterization of the previously unknown material LaCaScIrO$_6$ is reported. LaCaScIrO$_6$ presents a new example of the rare case of a double perovskite with the strongly spin-orbit coupled 5\textit{d}-ion Ir$^{4+}$ as its only magnetic species, forming a monoclinically distorted version of the frustrated fcc lattice. Magnetization measurements show a weak anomaly at 8~K. The Curie-Weiss temperature Θ$_{CW}$ and effective magnetic moment μ$_{eff}$ of LaCaScIrO$_6$ are in close proximity to the related compound La$_2$MgIrO$_6$ but differ from La$_2$ZnIrO$_6$. This suggests …
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…
Using detailed synchrotron diffraction, magnetization, thermodynamic and transport measurements, we investigate the relationship between the mixed valence of Ir, lattice strain and the resultant structural and magnetic ground states in the geometrically frustrated triple perovskite iridate Ba$_{3}$NaIr$_{2}$O$_{9}$. We observe a complex interplay between lattice strain and structural phase co-existence, which is in sharp contrast to what is typically observed in this family of compounds. The low temperature magnetic ground state is characterized by the absence of long range order, and points t…
Analogs of the high-T$_c$ cuprates have been long sought after in transition metal oxides. Due to the strong spin-orbit coupling (SOC), the $5d$ perovskite iridates Sr$_2$IrO$_4$ exhibit a low-energy electronic structure remarkably similar to the cuprates. Whether a superconducting state exists as in the cuprates requires understanding the correlated spin-orbit entangled electronic states. Recent experiments discovered hidden order in the parent and electron doped iridates, some with striking analogies to the cuprates, including Fermi surface pockets, Fermi arcs, and pseudogap. Here, we study …
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…
Perovskite iridates of 6H hexagonal structure present a plethora of possibilities in terms of the variety of ground states resulting from a competition between spin-orbit coupling (SOC), hopping, noncubic crystal field ($Δ_{CFE}^{NC}$) and superexchange energy scales within the Ir$_2$O$_9$ dimers. Here we have investigated one such compound Ba$_3$CdIr$_2$O$_9$ by x-ray diffraction, dc magnetic susceptibility($χ$), heat capacity($C_p$) and also ${}^{113}$Cd nuclear magnetic resonance (NMR) spectroscopy. We have established that the magnetic ground state has a small but finite magnetic moment on…
We report electron spin resonance (ESR) spectroscopy results on the double perovskite Ba$_2$YIrO$_6$. On general grounds, this material is expected to be nonmagnetic due to the strong coupling of the spin and orbital momenta of Ir$^{5+}$ (5$d^4$) ions. However, controversial experimental reports on either strong antiferromagnetism with static order at low temperatures or just a weakly paramagnetic behavior have triggered a discussion on the breakdown of the generally accepted scenario of the strongly spin-orbit coupled ground states in the 5$d^4$ iridates and the emergence of a novel exotic ma…
We present an analysis of the electronic structure of perovskite-related iridates, 5d electron compounds where a subtle interplay between spin-orbit coupling, tetragonal distortions and electron correlations determines the electronic structure properties. We suggest via electronic structure calculations that a non-collinear calculation is required to obtain solutions close to the usually quoted $j_{eff}$ = 1/2 state to describe the $t_{2g}$ hole in the $Ir^{4+} :d^5$ cation, while a collinear calculation yields a different solution, the hole is in a simpler xz/yz complex combination with a sma…
We report on our investigation on the magnetism of the iridate double perovskite Sr$_2$CoIrO$_6$, a nominally Ir$^{5+}$ Van Vleck $J_{eff}=0$ system. Using x-ray absorption (XAS) and x-ray magnetic circular dichroism (XMCD) spectroscopy at the Ir-$L_{2,3}$ edges, we found a nearly zero orbital contribution to the magnetic moment and thus an apparent breakdown of the $J_{eff}=0$ ground state. By carrying out also XAS and XMCD experiments at the Co-$L_{2,3}$ edges and by performing detailed full atomic multiplet calculations to simulate all spectra, we discovered that the compound consists of ab…
We theoretically investigate the mechanism to generate large intrinsic spin Hall effect in iridates or more broadly in 5d transition metal oxides with strong spin-orbit coupling. We demonstrate such a possibility by taking the example of orthorhombic perovskite iridate with nonsymmorphic lattice symmetry, SrIrO$_3$, which is a three-dimensional semimetal with nodal line spectrum. It is shown that large intrinsic spin Hall effect arises in this system via the spin-Berry curvature originating from the nearly degenerate electronic spectra surrounding the nodal line. This effect exists even when t…
Iridate oxides display exotic physical properties that arise from the interplay between a large spin-orbit coupling and electron correlations. Here, we present a comprehensive study of the effects of hydrostatic pressure on the electronic transport properties of SrIrO3 (SIO), a system that has recently attracted a lot of attention as potential correlated Dirac semimetal. Our investigations on untwinned thin films of SIO reveal that the electrical resistivity of this material is intrinsically anisotropic and controlled by the orthorhombic distortion of the perovskite unit cell. These effects pr…
We report a comprehensive investigation of the triple perovskite iridate Ba$_{3}$CoIr$_{2}$O$_{9}$. Stabilizing in the hexagonal $P6_{3}/mmc$ symmetry at room temperature, this system transforms to a monoclinic $C2/c$ symmetry at the magnetic phase transition. On further reduction in temperature, the system partially distorts to an even lower symmetry ($P2/c$), with both these structurally disparate phases coexisting down to the lowest measured temperatures. The magnetic structure as determined from neutron diffraction data indicates a weakly canted antiferromagnetic structure, which is also s…
Perovskite SrIrO3 has long been proposed as an exotic semimetal induced by the interplay between the spin-orbit coupling and electron correlations. However, its low-lying electronic structure is still lacking. We synthesize high-quality perovskite SrIrO3 (100) films by means of oxide molecular beam epitaxy, and then systemically investigate their low energy electronic structure using in-situ angle-resolved photoemission spectroscopy. We find that the hole-like bands around R and the electron-like bands around U(T) intersect the Fermi level simultaneously, providing the direct evidence of the s…
We investigated the electronic properties of epitaxially stabilized perovskite SrIrO3 and demonstrated the effective strain-control on its electronic structure. Comprehensive transport measurements showed that the strong spin-orbit coupling renders a novel semimetallic phase for the J_eff=1/2 electrons rather than an ordinary correlated metal, elucidating the nontrivial mechanism underlying the dimensionality-controlled metal-insulator transition in iridates. The electron-hole symmetry of this correlated semimetal was found to exhibit drastic variation when subject to bi-axial strain. Under co…
Evolution of effective magnetic exchange interaction under spin dilution in SrIr$_{1-x}$Sn$_x$O$_3$
School of Physical Science and Technology, ShanghaiTech University（上海科技大学物理科学与技术学院）；Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；Center for Transformative Science, ShanghaiTech University（上海科技大学变革科学中心）
Hybrid transition metal oxides continue to attract attention due to their multiple degrees of freedom ($e.g.$, lattice, charge, spin, and orbital) and versatile properties. Here we investigate the magnetic and electronic properties of the newly synthesized double perovskite Ba$_2$NiIrO$_6$, using crystal field theory, superexchange model analysis, density functional calculations, and parallel tempering Monte Carlo (PTMC) simulations. Our results indicate that Ba$_2$NiIrO$_6$ has the Ni$^{2+}$ ($t_{2g}^{6}e_{g}^{2}$)-Ir$^{6+}$ ($t_{2g}^{3}$) charge states. The first nearest-neighboring (1NN) Ni…
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 path from a Mott insulating phase to high temperature superconductivity encounters a rich set of unconventional phenomena involving the insulator-to-metal transition (IMT) such as emergent electronic orders and pseudogaps that ultimately affect the condensation of Cooper pairs. A huge hindrance to understanding the origin of these phenomena in the curates is the difficulty in accessing doping levels near the parent state. Recently, the J$_{eff}$=1/2 Mott state of the perovskite strontium iridates has revealed intriguing parallels to the cuprates, with the advantage that it provides unique …
