The 5$d$ based SrIrO$_3$ represents prototype example of nonmagnetic correlated metal which mainly originates from a combined effect of spin-orbit coupling, lattice dimensionality and crystal structure. Therefore, tuning of these parameters results in diverse physical properties in this material. Here, we study the structural, magnetic and electrical transport behavior in epitaxial SrIrO$_3$ film ($\sim$ 40 nm) grown on SrTiO$_3$ substrate. Opposed to bulk material, the SrIrO$_3$ film exhibits a ferromagnetic ordering at low temperature below $\sim$ 20 K. The electrical transport data indicate an insulating behavior where the nature of charge transport follows Mott's variable-range-hopping model. A positive magnetoresistance is recorded at 2 K which has correlation with magnetic moment. We further observe a nonlinear Hall effect at low temperature ($<$ 20 K) which arises due to an anomalous component of Hall effect. An anisotropic behavior of both magnetoresistance and Hall effect has been evidenced at low temperature which coupled with anomalous Hall effect indicate the development of ferromagnetic ordering. We believe that an enhanced (local) structural distortion caused by lattice strain at low temperatures induces ferromagnetic ordering, thus showing structural instability plays vital role to tune the physical properties in SrIrO$_3$.
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…
We investigate the effects of compressive strain on the electrical resistivity of 5d iridium based perovskite SrIrO3 by depositing epitaxial films of thickness 35 nm on various substrates such as GdScO3 (110), DyScO3 (110), and SrTiO3 (001). Surprisingly, we find anomalous transport behaviors in the tempeature dependent resistivity, where the temperature exponent evolves continuously from 4/5 to 1 and to 3/2 with an increase of compressive strain. Furthermore, magnetoresistance always remains positive irrespective of resistivity upturns at low temperatures. These observations imply that the de…
5d transition-metal-based oxides display emergent phenomena due to the competition between the relevant energy scales of the correlation, bandwidth, and most importantly, the strong spin-orbit coupling (SOC). Starting from the prediction of novel oxide topological insulators in bilayer ABO3 (B = 5d elements) thin-film grown along the (111) direction, 5d-based perovskites (Pv) form a new paradigm in the thin-film community. Here, we reviewed the scientific accomplishments in Pv-SrIrO3 thin films, a popular candidate for observing non-trivial topological phenomena. Although the predicted topolog…
SrIrO$_3$ crystallizes in a monoclinic structure of distorted hexagonal perovskite at ambient pressure. The transport measurements show that the monoclinic SrIrO$_3$ is a low-carrier density semimetal, as in the orthorhombic perovskite polymorph. The electronic structure calculation indicates a semimetallic band structure with Dirac bands at two high-symmetry points of Brillouin zone only when spin-orbit coupling is incorporated, suggesting that the semimetallic state is produced by the strong spin-orbit coupling. We argue that the Dirac bands are protected by the non-symmorphic symmetry of la…
Understanding of metal insulator transitions in a strongly correlated system, driven by Anderson localization (disorder) and/or Mott localization (correlation), is a long standing problem in condensed matter physics. The prevailing fundamental question would be how these two mechanisms contrive to accomplish emergent anomalous behaviors. Here, we have grown high quality perovskite SrIrO3 thin films, containing a strong spin orbit coupled 5d element Ir, on various substrates such as GdScO3 (110), DyScO3 (110), SrTiO3 (001), and NdGaO3 (110) with increasing lattice mismatch, in order to carry ou…
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…
Ab initio study of $Z_2$ topological phases in perovskite (111) $(\text{SrTiO}_3)_7/(\text{SrIrO}_3)_2$ and $(\text{KTaO}_3)_7/(\text{KPtO}_3)_2$ multilayers
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…
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…
Artificially fabricated 3$d$/5$d$ superlattices (SLs) involve both strong electron correlation and spin-orbit coupling in one material by means of interfacial 3$d$-5$d$ coupling, whose mechanism remains mostly unexplored. In this work we investigated the mechanism of interfacial coupling in LaMnO$_3$/SrIrO$_3$ SLs by several spectroscopic approaches. Hard x-ray absorption, magnetic circular dichroism and photoemission spectra evidence the systematic change of the Ir ferromagnetism and the electronic structure with the change of the SL repetition period. First-principles calculations further re…
Electron-boson interaction is fundamental to a thorough understanding of various exotic properties emerging in many-body physics. In photoemission spectroscopy, photoelectron emission due to photon absorption would trigger diverse collective excitations in solids, including the emergence of phonons, magnons, electron-hole pairs, and plasmons, which naturally provides a reliable pathway to study electron-boson couplings. While fingerprints of electron-phonon/-magnon interactions in this state-of-the-art technique have been well investigated, much less is known about electron-plasmon coupling, a…
The 5d iridium-based transition metal oxides have gained broad interest because of their strong spin-orbit coupling which favors new or exotic quantum electronic states. On the other hand, they rarely exhibit more mainstream orders like ferromagnetism due to generally weak electron-electron correlation strength. Here, we show a proximity-induced ferromagnetic (FM) state with TC = 100 K and strong magnetocrystalline anisotropy in a SrIrO3 (SIO) heterostructure via interfacial charge transfer by using a ferromagnetic insulator in contact with SIO. Electrical transport allows to selectively probe…
Perovskite-type iridates SrIrO$_{3}$ and CaIrO$_{3}$ are a Dirac line node semimetal protected by crystalline symmetry, providing an interesting playground to investigate electron correlation effects on topological semimetals. The effect of Sn doping was examined by growing SrIr$_{1-x}$Sn$_{x}$O$_{3}$ and CaIr$_{1-x}$Sn$_{x}$O$_{3}$ thin films epitaxially on SrTiO$_{3}$(001) substrate using pulsed laser deposition. Upon Sn doping, the semimetallic ground state switches into an insulator. As temperature is lowered, the resistivity, $ρ(T)$, of SrIr$_{1-x}$Sn$_{x}$O$_{3}$ above a critical doping …
We carry out a first-principles investigation on magnetism, electronic structure, magneto-optical effects and topological property of newly grown cubic double perovskite Ba2NiOsO6 and its (111) (Ba2NiOsO6)/(BaTiO3)10 superlattice, based on the density functional theory with the generalized gradient approximation (GGA) plus onsite Couloumb interactions. Interestingly, we find that both structures are rare ferromagnetic (FM) semiconductors with estimated Curie temperatures of ~150 and 70 K, respectively. The calculated near-neighbor exchange coupling parameters reveal that the ferromagnetism is …
To investigate the relationship between the charge redistribution and ferromagnetism at the heterointerface between perovskite transition-metal oxides LaNiO$_3$ (LNO) and LaMnO$_3$ (LMO), we performed x-ray absorption spectroscopy and x-ray magnetic circular dichroism (XMCD) measurements. In the LNO/LMO heterostructures with asymmetric charge redistribution, the electrons donated from Mn to Ni ions are confined within one monolayer (ML) of LNO at the interface, whereas holes are distributed over 3-4 ML on the LMO side. A detailed analysis of the Ni-$L_{2,3}$ and Mn-$L_{2,3}$ XMCD spectra revea…
Perovskite SrIrO3 (SIO) films epitaxially deposited with a thickness of about 60 nm on various substrate materials display nearly strain-relieved state. Films grown on orthorhombic (110) DyScO3 (DSO) are found to display untwinned bulk-like orthorhombic structure. However, film deposition on cubic (001) SrTiO3 induces a twinned growth of SIO. Resistance measurements on the SIO films reveal only weak temperature dependence, where the resistance R increases with decreasing temperature T. Hall measurements show dominant electron-like transport throughout the temperature range from 2 K to 300 K. A…
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…
Inducing ferromagnetism by structural engineering in a strongly spin-orbit coupled oxide
Universität Würzburg（维尔茨堡大学）；International Research Centre MagTop, Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所磁顶国际研究中心）；CNR-SPIN, UOS Salerno（萨莱诺国家研究委员会自旋单元）；Leibniz Institute for Solid State and Materials Research Dresden（德累斯顿莱布尼兹固体与材料研究所）；TU Dresden（德累斯顿工业大学）；Synchrotron SOLEIL（索雷尔同步辐射中心）
We performed in-situ angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES (SARPES) experiments to investigate the relationship between electronic band structures and ferromagnetism in SrRuO$_3$ (SRO) thin films. Our high-quality ARPES and SARPES results show clear spin-lifted band structures. The spin polarization is strongly dependent on momentum around the Fermi level, whereas it becomes less dependent at high-binding energies. This experimental observation matches our dynamical mean-field theory (DMFT) results very well. As temperature increases from low to the Curie te…
The puzzling observation of room temperature ferromagnetism in double perovskites (A$_2$BB$'$O$_6$), despite having the magnetic lattice of B-ions diluted by non-magnetic B$'$-ions, have been examined for Sr$_2$FeReO$_6$. {\it Ab-initio} spin spiral electronic structure calculations along various high symmetry directions in reciprocal space are used to determine the exchange interactions entering an extended Heisenberg model, which is then solved classically using Monte Carlo simulations to determine the ferromagnetic transition temperature T$_c$. We find that one must consider onsite Coulomb …
Perovskite SrRuO$_3$ is a prototypical itinerant ferromagnet which allows interface engineering of its electronic and magnetic properties. We report synthesis and investigation of atomically flat artificial multilayers of SrRuO$_3$ with the spin-orbit semimetal SrIrO$_3$ in combination with band-structure calculations with a Hubbard $U$ term and topological analysis. They reveal an electronic reconstruction and emergence of flat Ru-4d$_{xz}$ bands near the interface, ferromagnetic interlayer coupling and negative Berry-curvature contribution to the anomalous Hall effect. We analyze the Hall ef…
We investigate the unusual phase transitions in SrRuO$_{3}$ and Sr$_{0.5}$Ca$_{0.5}$Ru$_{1-x}$Cr$_{x}$O$_{3}$ (x=0,0.05 and 0.1) employing x-ray diffraction, resistivity, magnetic studies and x-ray photoemission spectroscopy. Our results show the compounds undergo crossover from $itinerant$ ferromagnetism to $localised$ ferromagnetism. The combined studies suggests Ru and Cr to be in 4+ valence state. A Griffith phase and an enhancement in Curie temperature (Tc) from 38 K to 107 K is observed with Cr doping. A shift in the chemical potential towards the valence band is observed with Cr doping.…
Single monolayer ferromagnetic perovskite SrRuO3 with high conductivity and strong ferromagnetism
NTT Basic Research Laboratories, NTT Corporation（NTT基础实验室，NTT公司）；The University of Tokyo（东京大学）；Hiroshima University（广岛大学）；Japan Synchrotron Radiation Research Institute (JASRI)（日本同步辐射研究所）
The ferromagnetic semiconductor Ba2NiOsO6 (Tmag ~100 K) was synthesized at 6 GPa and 1500 °C. It crystallizes into a double perovskite structure [Fm-3m; a = 8.0428(1) Å], where the Ni2+ and Os6+ ions are perfectly ordered at the perovskite B-site. We show that the spin-orbit coupling of Os6+ plays an essential role in opening the charge gap. The magnetic state was investigated by density functional theory calculations and powder neutron diffraction. The latter revealed a collinear ferromagnetic order in a >21 kOe magnetic field at 5 K. The ferromagnetic gapped state is fundamentally different …
The $4d$ and $5d$ transition metal oxides have become important members of the emerging quantum materials family due to competition between onsite Coulomb repulsion ($U$) and spin-orbit coupling (SOC). Specifically, the systems with $d^5$ electronic configuration in an octahedral environment are found to be capable of posessing invariant semimetallic state and perturbations can lead to diverse magnetic phases. In this work, by formulating a multi-band Hubbard model and performing SOC tunable DFT+$U$ calculations on a prototype SrIrO$_3$ and extending the analysis to other iso-structural and is…
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$_…
Impact of the Fe Doping on Magnetism in Perovskite Cobaltites
系统地研究了Fe掺杂钙钛矿型钴酸盐多晶样品：Pr $_{1-y}$ Ca $_{y}$ Co $_{1-x}$ Fe $_x$ O $_3$（$y$ =0.3，$x$ =0-0.15; $y$ =0.45，$x$ =0-0.3）和Gd $_{0.55}$ Sr $_{0.45}$ Co $_{1-x}$ Fe $_x$ O $_{3}$（$x$ =0-0.3）的磁性和输运性质。Fe掺杂使Pr $_{1-y}$ Ca $_{y}$ Co $_{1-x}$ Fe $_x$ O $_3$体系的铁磁性增强，但铁磁性随Fe含量的进一步增加而被抑制，在高Fe掺杂水平下观察到自旋玻璃行为。相反，只要Fe被掺杂，在系统Gd $_{0.55}$ Sr $_{0.45}$ Co $_{1-x}$ Fe $_x$ O $_{3}$中的铁磁性被抑制，并且在Fe掺杂高达0.3的样品中没有观察到自旋玻璃行为。通过Fe $^{3+}$ -O-（LS）Co $^{4+}$的铁磁相互作用与通过Fe $^{3+}$ -O-Fe $^{3+}$和Fe $^{3+}$ -O-（IS）Co $^{3+}$的反铁磁相互作用之间的竞争被认为是上述行为的原因。A位上离子的平均半径在确定Fe掺杂主要引入哪种类型的相互作用方面起着关键作用。
Multiferroicity and magnetodielectric coupling in metal-organic-frameworks (MOFs) is rare and so far restricted mainly to formate-based systems with perovskite structure. In the course of this work we designed a tetragonal framework [Co(C16H15N5O2)], exhibiting spin-chains of Co2+ ions, which are bridged by an organic linker containing a dipolar nitrobenzene moiety. This compound shows relaxor-like ferroelectricity at 100 K, which is followed by the onset of complex magnetic order at 15 K, indicative of weak ferromagnetism. The clear anomaly of the dielectric constant at the magnetic ordering …
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 have synthesized and characterized laser-deposited film samples of perovskite BaCrO_{3}, a missing member of the perovskite-chromate family. The BaCrO_{3} films have a substantially larger lattice constant than other chromates, are insulating, and exhibit weak ferromagnetism likely associated with canted antiferromagnetism. Comparison with the other sister compounds CaCrO_{3} and SrCrO_{3} suggest an anomalous Mott transition where magnetism is independent of whether the compound is metallic or insulating
Strong Coulomb repulsion and spin-orbit coupling are known to give rise to exotic physical phenomena in transition metal oxides. Initial attempts to investigate systems where both of these fundamental interactions are comparably strong, such as 3d and 5d complex oxide superlattices, have revealed properties that only slightly differ from the bulk ones of the constituent materials. Here, we observe that the interfacial coupling between the 3d antiferromagnetic insulator SrMnO3 and the 5d paramagnetic metal SrIrO3 is enormously strong, yielding an anomalous Hall response as the result of charge …
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 …
We study from first principles the magnetic, electronic, orbital and structural properties of the LaMnO3 doped with gallium replacing the Mn-site. The gallium doping reduces the Jahn-Teller effect, and consequently the bandgap. Surprisingly, the system does not go towards a metallic phase because of the Mn-bandwidth reduction. The Ga-doping tends to reduce the orbital order typical of bulk antiferromagnetic LaMnO3 and consequently weakens the antiferromagnetic phase. The Ga-doping favors the G-type orbital order and layered-ordered ferromagnetic perovskite at x=0.50, both effects contribute to…
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…
High-Pressure Tuning of Electrical Transport in Freestanding Oxide Films
Anhui Provincial Key Laboratory of Low-Energy Quantum Materials and Devices, High Magnetic Field Laboratory, HFIPS, Chinese Academy of Sciences（中国科学院合肥物质科学研究院、安徽省低能量子材料与器件重点实验室）；Science Island Branch of Graduate School, University of Science and Technology of China（中国科学技术大学研究生院科学岛分部）；School of Microelectronics and Control Engineering, Changzhou University（常州大学微电子与控制工程学院）；Spin-X Institute, School of Chemistry and Chemical Engineering, South China University of Technology（华南理工大学化学与化工学院自旋X研究所）
The perovskite rare-earth titanates are model Mott insulators with magnetic ground states that are very sensitive to structural distortions. These distortions couple strongly to the orbital degrees of freedom and, in principle, it should be possible to tune the superexchange and the magnetic transition with strain. We investigate the representative system (Y,La,Ca)TiO$_3$, which exhibits low crystallographic symmetry and no structural instabilities. From magnetic susceptibility measurements of the Curie temperature, we demonstrate direct, reversible and continuous control of ferromagnetism by …
