Evolution of magnetic phases and orbital occupation in (SrMnO3)n/(LaMnO3)2n superlattices
C. Aruta, C. Adamo, A. Galdi, P. Orgiani, V. Bisogni, N. B. Brookes, J. C. Cezar, P. Thakur, C. A. Perroni, G. De Filippis, V. Cataudella, D. G. Schlom, L. Mari… 展开作者
C. Aruta, C. Adamo, A. Galdi, P. Orgiani, V. Bisogni, N. B. Brookes, J. C. Cezar, P. Thakur, C. A. Perroni, G. De Filippis, V. Cataudella, D. G. Schlom, L. Maritato, G. Ghiringhelli
备注：
accepted for publication as a Rapid Communication in Physical Review B
The magnetic and electronic modifications induced at the interfaces in (SrMnO$_{3}$)$_{n}$/(LaMnO$_{3}$)$_{2n}$ superlattices have been investigated by linear and circular magnetic dichroism in the Mn L$_{2,3}$ x-ray absorption spectra. Together with theoretical calculations, our data demonstrate that the charge redistribution across interfaces favors in-plane ferromagnetic (FM) order and $e_{g}(x^{2}-y^{2})$ orbital occupation, in agreement with the average strain. Far from interfaces, inside LaMnO$_3$, electron localization and local strain favor antiferromagnetism (AFM) and $e_{g}(3z^{2}-r^{2})$ orbital occupation. For $n=1$ the high density of interfacial planes ultimately leads to dominant FM order forcing the residual AFM phase to be in-plane too, while for $n \geq 5$ the FM layers are separated by AFM regions having out-of-plane spin orientation.
X-ray absorption spectroscopy and resonant soft x-ray reflectivity show a non-uniform distribution of oxygen holes in a La2NiO4 - La2CuO4 (LNO-LCO) superlattice, with excess holes concentrated in the LNO layers. Weak ferromagnetism with Tc = 160 K suggests a coordinated tilting of NiO6 octahedra, similar to that of bulk LNO. Ni d3z2-r2 orbitals within the LNO layers have a spatially variable occupation. This variation of the Ni valence near LNO-LCO interfaces is observed with resonant soft x-ray reflectivity at the Ni L edge, at a reflection suppressed by the symmetry of the structure, and is …
Manipulating the orbital state in a strongly correlated electron system is of fundamental and technological importance for exploring and developing novel electronic phases. Here, we report an unambiguous demonstration of orbital occupancy control between t2g and eg multiplets in quasi-twodimensional transition metal oxide superlattices (SLs) composed of a Mott insulator LaCoO3 and a band insulator LaAlO3. As the LaCoO3 sublayer thickness approaches its fundamental limit (i.e. one unit-cell-thick), the electronic state of the SLs changed from a Mott insulator, in which both t2g and eg orbitals …
A combined analysis of x-ray absorption and resonant reflectivity data was used to obtain the orbital polarization profiles of superlattices composed of four-unit-cell-thick layers of metallic LaNiO3 and layers of insulating RXO3 (R=La, Gd, Dy and X=Al, Ga, Sc), grown on substrates that impose either compressive or tensile strain. This superlattice geometry allowed us to partly separate the influence of epitaxial strain from interfacial effects controlled by the chemical composition of the insulating blocking layers. Our quantitative analysis reveal orbital polarizations up to 25%. We further …
The two-orbital double-exchange model is employed for the study of the magnetic and orbital orders in ($R$MnO$_3$)$_n$/($A$MnO$_3$)$_{2n}$ ($R$: rare earths; $A$: alkaline earths) superlattices. The A-type antiferromagnetic order is observed in a broad region of parameter space for the case of SrTiO$_3$ as substrate, in agreement with recent experiments and first-principles calculations using these superlattices. In addition, also a C-type antiferromagnetic state is predicted to be stabilized when using substrates like LaAlO$_3$ with smaller lattice constants than SrTiO$_3$, again in agreement…
The effects of lattice relaxation in LaTiO$_3$/SrTiO$_3$ superlattices are investigated using a combination of LDA$+U$ density functional theory, and Hartree-Fock effective Hamiltonian calculations. We find noticeable ($\sim 0.1$--0.2 Å) distortions of the TiO$_6$ octahedra in the near-La region. The resulting screening changes the Ti $d$-electron density substantially. Tight-binding fits to the relaxed-lattice band structure, combined with Hartree-Fock calculations of the resulting model, reveal a novel phase with $xy$ orbital order, which does not occur in bulk LaTiO$_3$, or in the hypotheti…
We theoretically investigate topological properties of the one-dimensional superlattice anyon-Hubbard model, which can be mapped to a superlattice bose-Hubbard model with an occupation-dependent phase factor by fractional Jordan-Wigner transformation. The topological anyon-Mott insulator is identified by topological invariant and edge modes using exact diagonalization and density-matrix renormalization-group algorithm. When only the statistical angle is varied and all other parameters are fixed, a statistically induced topological phase transition can be realized, which provides new insights i…
Dynamical mean field methods are used to calculate the phase diagram, many-body density of states, relative orbital occupancy and Fermi surface shape for a realistic model of $LaNiO_3$-based superlattices. The model is derived from density functional band calculations and includes oxygen orbitals. The combination of the on-site Hunds interaction and charge-transfer between the transition metal and the oxygen orbitals is found to reduce the orbital polarization far below the levels predicted either by band structure calculations or by many-body analyses of Hubbard-type models which do not expli…
Metal-insulator transition was microscopically investigated by orbital-resolved nuclear magnetic resonance (OR-NMR) spectroscopy in a single crystal of vanadium dioxide VO$_2$. Observations of the anisotropic $^{51}$V Knight shift and the nuclear quadrupole frequency allow us to evaluate orbital-dependent spin susceptibility and $d$ orbital occupations. The result is consistent with the degenerated $t_{2g}$ orbitals in a correlated metallic phase and the $d$ orbital ordering in a nonmagnetic insulating phase. The predominant orbital pointing along the chain facilitates a spin-singlet formation…
Novel interplay of spin-orbit coupling and electron correlations in complex Ir oxides recently emerged as a new paradigm for correlated electron physics. Because of a large spin-orbit coupling of ~0.5 eV, which is comparable to the transfer energy t and the crystal field splitting $Δ$ and Coulomb U, a variety of ground states including magnetic insulator, band insulator, semimetal and metal, shows up in a narrow materials phase space. Utilizing such subtle competition of the ground states, we successfully tailor a spin-orbital magnetic insulator out of a semimetal SrIrO$_3$ by controlling dime…
The interface electronic structure of correlated LaTiO$_3$/SrTiO$_3$ superlattices is investigated by means of the charge self-consistent combination of the local density approximation (LDA) to density functional theory (DFT) with dynamical mean-field theory (DMFT). Utilizing a pseudopotential technique together with a continuous-time quantum Monte-Carlo approach, the resulting complex multiorbital electronic states are addressed in a coherent fashion beyond static mean-field. General structural relaxations are taken into account on the LDA level and cooperate with the driving forces from stro…
We determine the phase diagram of a bilayer, Yao-Lee spin-orbital model with inter-layer interactions (J), for several stackings and moiré superlattices. For AA stacking, a gapped Z2 quantum spin liquid phase emerges at a finite Jc. We show that this phase survives in the well-controlled large-J limit, where an isotropic honeycomb toric code emerges. For moiré superlattices, a finite-q inter-layer hybridization is stabilized. This connects inequivalent Dirac points, effectively `untwisting' the system. Our study thus provides insight into the spin-liquid phases of bilayer spin-orbital Kitaev m…
Density functional band calculations have been performed to study LaNiO$_3$/LaAlO$_3$ superlattices. Motivated by recent experiments reporting the magnetic and metal-insulator phase transition as a function of LaNiO$_3$ layer thickness, we examined the electronic structure, magnetic properties, and orbital occupation depending on the number of LaNiO$_3$ layers. Calculations show that the magnetic phase is stabler than the nonmagnetic for finite and positive $U$ values. The orbital polarization is significantly reduced by $U$ even in the magnetic regions. The implications of the results are dis…
We report equations of motion for the occupation numbers of natural spin orbitals and show that adiabatic extensions of common functionals employed in ground-state reduced-density-matrix-functional theory have the shortcoming of leading always to occupation numbers which are independent of time. We illustrate the exact time-dependence of the natural spin orbitals and occupation numbers for the case of electron-ion scattering and for atoms in strong laser fields. In the latter case, we observe strong variations of the occupation numbers in time.
Large magnetoelectric response in thin films is highly desired for high-throughput and high-density microelectronic applications. However, the d0 rule in single-phase compounds usually results in a weak interaction between ferroelectric and magnetic orders; the magnetoelectric coupling via elastic resonance in composites restricts their thin-film integration in broadband. Here, we effectuate a concurrence of ferroelectric-like and antiferromagnetic phase transitions in Sr2IrO4/SrTiO3 superlattices by artificial design periodically non-equivalent interfaces, where a maximum magnetoelectric coef…
In pursuit of rational control of orbital polarization, we present a combined experimental and theoretical study of single unit cell superlattices of the correlated metal LaNiO$_3$ and the band insulator LaAlO$_3$. Polarized x-ray absorption spectra show a distinct asymmetry in the orbital response under strain. A splitting of orbital energies consistent with octahedral distortions is found for the case of compressive strain. In sharp contrast, for tensile strain, no splitting is found although a strong orbital polarization is present. Density functional theory calculations including a Hubbard…
Layered oxide heterostructures are the new routes to tailor desired electronic and magnetic phases emerging from competing interactions involving strong correlation, orbital hopping, tunnelling and lattice coupling phenomena. Here, we propose a half-metal/insulator superlattice that intrinsically forms spin-polarized two-dimensional electron gas (2DEG) following a mechanism very different from the widely reported 2DEG at the single perovskite polar interfaces. From DFT$+U$ study on Sr$_2$FeMoO$_6$/La$_2$CoMnO$_6$ (001) superlattice, we find that a periodic quantum well is created along [001] w…
We propose two complementary design principles for engineering three-dimensional (3D) Weyl semimetals and superconductors in a layer-by-layer setup which includes even and odd parity orbitals in alternating layers - dubbed orbital selective superlattice. Such structure breaks mirror symmetry along the superlattice growth axis which, with the help of either a basal plane spin-orbit coupling or a spinless p+ip superconductivity, stabilizes a 3D Dirac node. To explore this idea, we develop a 3D generalization of Haldane model and a Bogoliubov-de-Gennes (BdG) Hamiltonian for the two cases, respect…
CaBaFe4O7 is a mixed-valent transition metal oxide having both Fe2+ and Fe3+ ions in tetrahedral coordination. Here we characterize its magnetic properties by magnetization measurements and investigate its local electronic structure using soft x-ray absorption spectroscopy at the Fe L2,3 edges, in combination with multiplet cluster and spin-resolved band structure calculations. We found that the Fe2+ ion in the unusual tetrahedral coordination is Jahn-Teller active with the high-spin e^2 (up) t2^3 (up) e^1 (down) configuration having a x^2-y^2-like electron for the minority spin. We deduce tha…
Atomically precise superlattices involving transition metal oxides provide a unique opportunity to engineer correlated electron physics using strain (modulated by choice of substate) and quantum confinement (controlled by layer thickness). Here we use the combination of density functional theory and dynamical mean field theory (DFT+DMFT) to study Ni E$_g$ $d$-orbital polarization in strained LaNiO$_3$/LaAlO$_3$ superlattices consisting of four layers of nominally metallic NiO$_2$ and four layers of insulating AlO$_2$ separated by LaO layers. The layer-resolved orbital polarization is calculate…
We have investigated the magnetic response of La0.7Sr0.3MnO3/SrRuO3 superlattices to biaxial in-plane strain applied in-situ. Superlattices grown on piezoelectric substrates of 0.72PbMg1/3Nb2/3O3-0.28PbTiO3(001) (PMN-PT) show strong antiferromagnetic coupling of the two ferromagnetic components. The coupling field of mu0HAF = 2.8 T is found to decrease by deltaHAF/delta epsilon ~ -520 mT %-1 under reversible biaxial strain mu0HAF at 80 K in a [La0.7Sr0.3MnO3(22)/SrRuO3(55)]15 superlattice. This reveals a significant strain effect on interfacial coupling. The applied in-plane compression enhanc…
The crystal structure of Ca_{2-x}Sr_xRuO_4 with 0.2 < x < 1.0 has been studied by diffraction techniques and by high resolution capacitance dilatometry as a function of temperature and magnetic field. Upon cooling in zero magnetic field below about 25 K the structure shrinks along the c-direction and elongates in the a, b planes (0.2 < x < 1.0), whereas the opposite occurs upon cooling at high-field (x = 0.2 and 0.5). These findings indicate an orbital rearrangement driven by temperature and magnetic field, which accompanies the metamagnetic transition in these compounds.
We propose a two-orbital Hubbard model on an emergent honeycomb lattice to describe the low-energy physics of twisted bilayer graphene. Our model provides a theoretical basis for studying metal-insulator transition, Landau level degeneracy lifting and unconventional superconductivity that are recently observed.
A hypothetical layered oxide La_2NiMO_6 where NiO_2 and MO_2 planes alternate along the c-axis of ABO_3 perovskite lattice is considered theoretically. Here, M denotes a trivalent cation Al, Ga,... such that MO_2 planes are insulating and suppress the c-axis charge transfer. We predict that correlated e_g electrons in the NiO_2 planes develop a planar x^2-y^2 orbital order driven by the reduced dimensionality and further supported by epitaxial strain from the substrate. Low energy electronic states can be mapped to a single-band t-t'-J model, suggesting favorable conditions for high-T_c superc…
We studied the charge-orbital ordering in the superlattice of charge-ordered insulating Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ and ferromagnetic metallic La$_{0.5}$Sr$_{0.5}$MnO$_3$ by resonant soft x-ray diffraction. A temperature-dependent incommensurability is found in the orbital order. In addition, a large hysteresis is observed that is caused by phase competition between insulating charge ordered and metallic ferromagnetic states. No magnetic phase transitions are observed in contrast to bulk, confirming the unique character of the superlattice. The deviation from the commensurate orbital order can…
Using first-principles density functional theory calculations, we investigated the effect of charge doping in a LaNiO$_3$/SrTiO$_3$ superlattice. The detailed analysis based on two different simulation methods for doping clearly shows that the electronic and structural properties change in a systematic way that the orbital polarization ({\it i.e.} relative occupation of two Ni-$e_g$ orbitals) is reduced and the Ni to apical oxygen distance enlarged as the number of doped electrons increases. Also, the rotation angles of the NiO$_6$/TiO$_6$ octahedra strongly and systematically depend on the do…
Using first-principles density functional theory calculations, we examined the ground state property of LaTiO$_3$/LaAlO$_3$ superlattice. Total energy calculations, taking account of the structural distortions, $U$ dependence, and exchange correlation functional dependence, show that the spin and orbital ground state can be controlled systematically by the epitaxial strain. In the wide range of strains, ferromagnetic spin and antiferro orbital ordering are stabilized, which is notably different from the previously reported ground state in titanate systems. By applying large tensile strains, th…
We study the magnetic resonant x-ray scattering (RXS) spectra around the $K$ edge of Cu in KCuF$_3$ on the basis of an {\em ab initio} calculation. We use the full-potential linearlized augmented plane wave method in the LDA$+U$ scheme, and introduce the lattice distortion as inputs of the calculation. We obtain finite intensity on magnetic superlattice spots, about three orders of magnitude smaller than on orbital superlattice spots, by taking account of the spin-orbit interaction (SOI). No intensity appears without the SOI, indicating that the intensity arises not from the spin polarization …
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 …
The exact formulation of multi-configuration density-functional theory (DFT) is discussed in this work. As an alternative to range-separated methods, where electron correlation effects are split in the coordinate space, the combination of Configuration Interaction methods with orbital occupation functionals is explored at the formal level through the separation of correlation effects in the orbital space. When applied to model Hamiltonians, this approach leads to an exact Site-Occupation Embedding Theory (SOET). An adiabatic connection expression is derived for the complementary bath functiona…
The standard way to find the orbital occupation of Jahn-Teller (JT) ions is to use structural data, with the assumption of a one-to-one correspondence between the orbital occupation and the associated JT distortion, e.g. in O6 octahedron. We show, however, that this approach in principle does not work for layered systems. Specifically, using the layered manganite La0.5Sr1.5MnO4 as an example, we found from our x-ray absorption measurements and theoretical calculations, that the type of orbital ordering strongly contradicts the standard local distortion approach for the Mn3+O6 octahedra, and th…
The efficiency of optical emitters can be dramatically enhanced by reducing the effective mode volume (the Purcell effect). Here we predict an analogous enhancement for electron-phonon (el-ph) scattering, achieved by compressing the electronic Wannier orbitals. Reshaping of Wannier orbitals is a prominent effect in graphene moiré superlattices (SLs) where the orbitals are tunable by the twist angle. A reduction of the orbital effective volume leads to an enhancement in the effective el-ph coupling strength, yielding the values considerably bigger than those known for pristine monolayer graphen…
Charge transfer and competing symmetry breaking drive orbital reconstruction and emergent ferromagnetism in insulating oxide superlattices
Indian Institute of Science（印度科学学院）；Deutsches Elektronen-Synchrotron DESY（德国电子同步加速器中心）；ALBA Synchrotron Light Source（阿尔巴同步辐射光源）；Advanced Photon Source, Argonne National Laboratory（阿贡国家实验室先进光子源）
Occupation numbers of natural orbitals capture the physics of strong electron correlations in momentum space. A Natural Orbital Density Functional Theory based on the antisymmetrized geminal product provides these occupation numbers and the corresponding electron momentum density. A practical implementation of this theory approximates the natural orbitals by the Kohn-Sham orbitals and uses a mean-field approach to estimate pairing amplitudes leading to corrections for the independent particle model. The method is applied to weakly doped $\mbox{La$_2$CuO$_4$}$.
Using first-principles calculations based on the density functional theory, we show a strong strain dependence of magnetic order in (LaMnO$_{3}$)$_n$/(SrMnO$_{3}$)$_{2n}$ (001) superlattices with $n=1,2$. The epitaxial strain lifts the degeneracy of Mn $e_{g}$ orbitals, thus inducing an inherent orbital order, which in turn strongly affects the ferromagnetic double exchange of itinerant $e_{g}$ electrons, competing with the antiferromagnetic superexchange of localized $t_{2g}$ electrons. For the case of tensile strain induced by SrTiO$_3$ (001) substrate, we find that the ground state is A-typ…
The iterative perturbation theory of the dynamical mean field theory is generalized to arbitrary electron occupation in case of multi-orbital Hubbard bands. We present numerical results of doubly degenerate Eg bands in a simple cubic lattice. The spectrum shows the electron ionization and affinity levels of different electron occupations. For sufficiently large Coulomb integral, a gap opens in the spectrum at integer filling of electrons and the system becomes insulator. The present scheme is easy to combine with the LSDA electronic structure theory.
We present results on spin and charge correlations in two-dimensional quantum dots as a function of increasing Coulomb strength (dielectric constant). We look specifically at the orbital occupation of both spin and charge. We find that charge and spin evolve separately, especially at low Coulomb strength. For the charge, we find that a hole develops in the core orbitals at strong Coulomb repulsion, invalidating the common segregation of confined electrons into an inert core and active valence electrons. For excitations, we find a total spin-projection $S_z = -1/2$ breaks apart into separate oc…
Resonant soft x-ray absorption measurements at the O K edge on a SrMnO3/LaMnO3 superlattice show a shoulder at the energy of doped holes, which corresponds to the main peak of resonant scattering from the modulation in the doped hole density. Scattering line shape at the Mn L3,2 edges has a strong variation below the ferromagnetic transition temperature. This variation has a period equal to half the superlattice superperiod and follows the development of the ferromagnetic moment, pointing to a ferromagnetic phase developing at the interfaces. It occurs at the resonant energies for Mn3+ and Mn4…
Heterostructuring provides different ways to manipulate the orbital degrees of freedom and to tailor orbital occupations in transition metal oxides. However, the reliable prediction of these modifications remains a challenge. Here, we present a detailed investigation of the relationship between the crystal and electronic structure in YVO$_3$-LaAlO$_3$ superlattices by combining ab initio theory, scanning transmission electron microscopy, and x-ray diffraction. Density functional theory simulations including an on-site Coulomb repulsion term, accurately predict the crystal structure and in conj…
We apply the dynamical mean field theory (DMFT) in the iterative perturbation theory(IPT) to doubly degenerate eg bands and triply degenerate tg bands on a simple cubic lattice and calculate the spectrum and optical conductivity in arbitrary electron occupation. The spectrum simultaneously shows the effects of multiplet structure and DMFT together with the electron ionization and affinity levels of different electron occupations, coherent peaks at the Fermi energy in the metallic phase and a gap at an integer filling of electrons for sufficiently large Coulomb U. We also calculate the critical…
Ruthenium-based perovskite systems are attractive because their Structural, electronic and magnetic properties can be systematically engineered. SrRuO$_3$/SrTiO$_3$ superlattice, with its period consisting of one unit cell each, is very sensitive to strain change. Our first-principles simulations reveal that in the high tensile strain region, it transits from a ferromagnetic (FM) metal to an antiferromagnetic (AFM) insulator with clear tilted octahedra, while in the low strain region, it is a ferromagnetic metal without octahedra tilting. Detailed analyses of three spin-down Ru-t$_{2g}$ orbita…
We have performed x-ray linear and circular magnetic dichroism experiments at the Mn L2,3-edge of the La0.7Sr0.3MnO3 ultra thin films. Our measurements show that the antiferromagnetic (AF) insulating phase is stabilized by the interfacial rearrangement of the Mn 3d orbitals, despite the relevant magnetostriction anisotropic effect on the double-exchange ferromagnetic (FM) metallic phase. As a consequence, the Mn atomic magnetic moment orientation and how it reacts to strain differ in the FM and AF phases. In some cases a FM insulating (FMI) phase adds to the AF and FM. Its peculiar magnetic pr…
Charge and orbital ordering behaviors in the half doped bi-layered compound LaSr2Mn2O7 have been studied by resonant and non-resonant X-ray scattering. Three different order parameters, which correspond to the A-type antiferromagnetic, a charge and an orbital ordered states, were observed by measuring the magnetostriction and the superlattice peaks characterized by wavevectors (1/2 1/2 0) and (1/4 1/4 0), respectively. The superlattice reflections indicating the charge and orbital ordered states were observed below 210 K. Both the intensities reach a maximum at 160 K on cooling and become very…
We discuss the possibility of a Kondo like effect associated with H in metals resulting from the strong dependence of the H1s orbital radius on the occupation number. We demonstrate that such a strong breathing property of the orbital radius, which translates directly into a strong occupation dependent hopping, results in the formation of local singlet-like bound states involving one electron on H and one on the surrounding metal orbitals. We also show that already at a mean field level an occupation dependent hopping integral leads to a substantial potential energy correction on hydrogen, and…
We present the results of an LDA and LDA+U band structure study of the monoclinic and the corundum phases of V2O3 and argue that the most prominent (spin 1/2) models used to describe the semiconductor metal transition are not valid. Contrary to the generally accepted assumptions we find that the large on site Coulomb and exchange interactions result in a total local spin of 1 rather than 1/2 and especially an orbital occupation which removes the orbital degeneracies and the freedom for orbital ordering. The calculated exchange interaction parameters lead to a magnetic structure consistent with…
Superlattices built from two antiferromagnetic (AFM) charge/orbital order compounds, $Pr_{0.5}Ca_{0.5}MnO_3$ and $La_{0.5}Ca_{0.5}MnO_3$, have been studied as the thickness of $La_{0.5}Ca_{0.5}MnO_3$ ($LCMO$) varied. High structural quality thin films were obtained on $LaAlO_3$ substrates using the pulsed laser deposition technique. An antiferromagnetic-to-ferromagnetic transition, in addition to an enhancement of the coercivity, are observed as the $LCMO$ layer thickness increases. The small shift in the origin of the field-cooled hysteresis loop along the field axis indicates the presence of…
Using Co-L_(2,3) and O-K x-ray absorption spectroscopy, we reveal that the charge ordering in La_(1.5)Sr_(0.5)CoO4 involves high spin (S=3/2) Co^2+ and low spin (S=0) Co^3+ ions. This provides evidence for the spin blockade phenomenon as a source for the extremely insulating nature of the La_(2-x)Sr_(x)CoO4 series. The associated e_g^2 and e_g^0 orbital occupation accounts for the large contrast in the Co-O bond lengths, and in turn, the high charge ordering temperature. Yet, the low magnetic ordering temperature is naturally explained by the presence of the non-magnetic (S=0) Co^3+ ions. From…
We use Quantum Monte Carlo simulations and exact diagonalization to explore the phase diagram of the Bose-Hubbard model with an additional superlattice potential. We first analyze the properties of superfluid and insulating phases present in the hard-core limit where an exact analytic treatment is possible via the Jordan-Wigner transformation. The extension to finite on-site interaction is achieved by means of quantum Monte Carlo simulations. We determine insulator/superfluid phase diagrams as functions of the on-site repulsive interaction, superlattice potential strength, and filling, finding…
A set of broken symmetry two-dimensional ground states are predicted in (111)-oriented (LaNiO$_3$)$_N$/(LaAlO$_3$)$_M$ ($N$/$M$) superlattices, based on density functional theory (DFT) calculations including a Hubbard $U$ term. An unanticipated Jahn-Teller distortion with $d_{z^2}$ orbital polarization and a FM Mott insulating (and multiferroic) phase emerges in the double perovskite (1/1), that shows strong susceptibility to strain-controlled orbital engineering. The LaNiO$_3$ bilayer with graphene topology has a switchable multiferroic (ferromagnetic (FM) and ferroelectric) insulating ground…
The density functional plus U method is used to obtain the electronic structure, lattice relaxation and metal-insulator phase diagram of superlattices consisting of $m$ layers of Gadolinium Titanate (GdTiO$_{3}$) alternating with $n$ layers of Strontium Titanate (SrTiO$_{3}$). Metallic phases occur when the number of SrTiO$_3$ layers is large or the interaction $U$ is small. In metallic phases, the mobile electrons are found in the SrTiO$_3$ layers, with near-interface electrons occupying $xy$-derived bands, while away from the interface the majority of electrons reside in $xz/yz$ bands. As th…
The unequal electronic occupation of localized orbitals (orbital polarization), and associated lowering of symmetry and degeneracy, play an important role in the properties of transition metal oxides. Here, we examine systematically the underlying origin of orbital polarization, taking as exemplar the 3$d$ manifold of Co$^{2+}$ in a variety of spin, orbital and structural phases in the double perovskite La$_2$CoTiO$_6$ and the (001) superlattice (LaCoO$_3$)$_1$+(LaTiO$_3$)$_1$ systems. Superlattices are of specific interest due to the large experimentally observed orbital polarization of their…
Chern insulator ferromagnets are characterized by a quantized anomalous Hall effect, and have so far been identified experimentally in magnetically-doped topological insulator (MTI) thin films and in bilayer graphene moir{é} superlattices. We classify Chern insulator ferromagnets as either spin or orbital, depending on whether the orbital magnetization results from spontaneous spin-polarization combined with spin-orbit interactions, as in the MTI case, or directly from spontaneous orbital currents, as in the moir{é} superlattice case. We argue that in a given magnetic state, characterized for …
Manipulating magnetic anisotropy (MA) purposefully in transition metal oxides (TMOs) enables the development of oxide-based spintronic devices with practical applications. Here, we report a pathway to reversibly switch the lateral magnetic easy-axis via interfacial oxygen octahedral coupling (OOC) effects in 3d-5d tricolor superlattices, i.e. [SrIrO3,mRTiO3,SrIrO3,2La0.67Sr0.33MnO3]10 (RTiO3: SrTiO3 and CaTiO3). In the heterostructures, the anisotropy energy (MAE) is enhanced over one magnitude to ~106 erg/cm3 compared to La0.67Sr0.33MnO3 films. Moreover, the magnetic easy-axis is reversibly r…
The origin of x-ray magnetic circular dichroism (XMCD) at the Cu L2,3 edge in YBa2Cu3O7/La(1-x)Ca(x)MnO3 superlattices is revealed by performing first-principle electronic structure calculation using fully-relativistic spin-polarized linear muffin-tin orbital and projected augmented plane wave methods. We show that the XMCD spectra at the Cu L2,3 edges are proportional to the difference of the densities of majority- and minority-spin Cu 3z2-1 states. Although the Cu 3z2-1 states lie well below the Fermi level, a small number of majority-spin 3z2-1 holes is created by the Cu 3z2-1 - O p_z - Mn …
The emergence of superlattice periodicities at metal to insulator transitions in hole doped perovskite oxides responds to a rearrangement of the local atomic structure, and electron and spin density distribution. Originally, the ionic model based on a checkerboard- type atomic distribution served to describe the low temperature charge and orbital ordered (COO) phases arising in half- doped manganites. In the last years, the exploitation of resonant x- ray scattering (RXS) capabilities has shown the need to revisit these concepts and improve the picture. Yet, we have realised that COO is a more…
We studied the magnetic properties of La$_{0.7}$Ca$_{0.3}$MnO$_3$ / YBa$_2$Cu$_3$O$_{7-δ}$ superlattices. Magnetometry showed that with increasing YBa$_2$Cu$_3$O$_{7-δ}$ layer thickness the saturation magnetization per La$_{0.7}$Ca$_{0.3}$MnO$_3$ layer decreases. From polarized neutron reflectometry we determined that this magnetization reduction is due to an inhomogenous magnetization depth profile arising from the suppression of magnetization near the La$_{0.7}$Ca$_{0.3}$MnO$_3$ / YBa$_2$Cu$_3$O$_{7-δ}$ interface. Electron energy loss spectroscopy indicates an increased 3d band occupation of…
The occupation of d-orbitals controls the magnitude and anisotropy of the inter-atomic electron transfer in transition metal oxides and hence exerts a key influence on their chemical bonding and physical properties. Atomic-scale modulations of the orbital occupation at surfaces and interfaces are believed to be responsible for massive variations of the magnetic and transport properties, but could thus far not be probed in a quantitative manner. Here we show that it is possible to derive quantitative, spatially resolved orbital polarization profiles from soft x-ray reflectivity data, without re…
Using first-principles density functional theory calculations, we investigated the electronic structure and magnetic properties of (LaMnO$_3$)$_m$/(LaNiO$_3$)$_n$ superlattices stacked along (001)-direction. The electrons are transferred from Mn to Ni, and the magnetic moments are induced at Ni sites that are paramagnetic in bulk and other types of superlattices. The size of induced moment is linearly proportional to the amount of transferred electrons, but it is larger than the net charge transfer because the spin and orbital directions play important roles and complicate the transfer process…
