Inspired by the experimental findings of an exotic ferromagnetic insulating state in LaMnO$_3$/SrTiO$_3$ heterostructures, we calculate the electronic and magnetic state of LaMnO$_3$/SrTiO$_3$ superlattices with comparable thicknesses employing ab-initio dynamical mean-field theory. Projecting on the low-energy subspace of Mn $3d$ and Ti $3d$ states, and solving a multi-impurity problem, our approach emphasizes on local correlations at Mn and Ti sites. We find that a ferromagnetic insulating state emerges due to intrinsic effects of strong correlations in the system, in agreement with experimental studies. We also predict that, due to electronic correlations, the emerging 2D electron gas is located at the LMO side of the interface. This is in contrast to DFT results that locate the electron gas on the STO side. We estimate the transition temperature for the paramagnetic to ferromagnetic phase transition, which may be verified experimentally. Importantly, we also clarify that the epitaxial strain is a key ingredient for the emergence of the exotic ferromagnetic insulating state. This becomes clear from calculations on a strained LaMnO$_3$ system, also showing ferromagnetism which is not seen in the unstrained bulk material.
We derive a spin-orbital model for insulating LaMnO_3 which fulfills the SU(2) symmetry of S=2 spins at Mn^{3+} ions. It includes the complete e_g and t_{2g} superexchange which follows from a realistic Mn^{2+} multiplet structure in cubic site symmetry, and the Jahn-Teller induced orbital interactions. We show that the magnetic ordering observed in LaMnO_3 is stabilized by a purely electronic mechanism due to the e_g-superexchange alone, and provide for the first time a quantitative explanation of the observed transition temperature and the anisotropic exchange interactions.
Motivated by the puzzling report of the observation of a ferromagnetic insulating state in LaMnO$_3$/SrTiO$_3$ heterostructures, we calculate the electronic and magnetic state of LaMnO$_3$, coherently matched to a SrTiO$_3$ square substrate within a "strained-bulk" geometry. We employ three different density functional theory based computational approaches: (a) density functional theory (DFT) supplemented with Hubbard U (DFT+U), (b) DFT + dynamical mean field theory (DMFT), and (c) a hybrid functional treatment of the exchange-correlation functional. While the first two approaches include loca…
The intrinsic magnetic state (ferromagnetic or antiferromagnetic) of ultra-thin LaMnO$_3$ films on the mostly used SrTiO$_3$ substrate is a long-existing question under debate. Either strain effect or non-stoichiometry was argued to be responsible for the experimental ferromagnetism. In a recent experiment [Science \textbf{349}, 716 (2015)], one more mechanism, namely the self-doping due to polar discontinuity, was argued to be the driving force of ferromagnetism beyond the critical thickness. Here systematic first-principles calculations have been performed to check these mechanisms in ultra-…
We report the effect of $δ$-doping at LaAlO$_{3}$/SrTiO$_{3}$ interface with LaMnO$_{3}$ monolayers on the photoconducting (PC) state. The PC is realized by exposing the samples to broad band optical radiation of a quartz lamp and 325 and 441 nm lines of a He-Cd laser. Along with the significant modification in electrical transport which drives the pure LaAlO$_{3}$/SrTiO$_{3}$ interface from metal-to-insulator with increasing LaMnO$_{3}$ sub-monolayer thickness, we also observe an enhancement in the photo-response and relaxation time constant. Possible scenario for the PC based on defect-clust…
Strongly correlated materials often exhibit an electronic phase separation (EPS) phenomena whose domain pattern is random in nature. The ability to control the spatial arrangement of the electronic phases at microscopic scales is highly desirable for tailoring their macroscopic properties and/or designing novel electronic devices. Here we report the formation of EPS nanoscale network in a mono-atomically stacked LaMnO3/CaMnO3/PrMnO3 superlattice grown on SrTiO3 (STO) (001) substrate, which is known to have an antiferromagnetic (AFM) insulating ground state. The EPS nano-network is a consequenc…
We have performed ab initio calculations within the LDA+U method in the multilayered system (LaMnO$_3$)$_{2n}$ / (SrMnO$_3$)$_n$. Our results suggest a charge-ordered state that alternates Mn$^{3+}$ and Mn$^{4+}$ cations in a checkerboard in-plane pattern is developed at the interfacial layer, leading to a gap opening. Such an interfacial charge-ordered situation would be the energetically favored reconstruction between LaMnO$_3$ and SrMnO$_3$. This helps understanding the insulating behavior observed experimentally in these multilayers at intermediate values of $n$, whose origin is known to b…
Here we investigate LaAlO_3-SrTiO_3 heterostructure withδ-doping of the interface by LaMnO_3 at less than one monolayer. This doping strongly inhibits the formation of mobile electron layer at the interface. This results in giant increase of the resistance and the thermopower of the heterostructure. Several aspects of this phenomena are investigated. A model to calculate the carrier concentration is presented and effect of doping and detailed temperature dependence is analyzed in terms of model parameters and the weak-scattering theory. The large enhancement of thermopower is attributed to the…
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…
Using neutron reflectometry and resonant x-ray techniques we studied the magnetic proximity effect (MPE) in superlattices composed of superconducting YBa$_2$Cu$_3$O$_7$ (YBCO) and ferromagnetic-metallic (FM-M) La$_{0.67}$Ca$_{0.33}$MnO$_{3}$ (LCMO) or ferromagnetic-insulating (FM-I) LaMnO$_{3+δ}$ (LMO). We find that the MPE strongly depends on the electronic state of the manganite layers, being pronounced for the FM-M LCMO and almost absent for FM-I LMO. We also detail the change of the magnetic depth profile due to the MPE and provide evidence for its intrinsic nature.
We have investigated the transport properties of LaVO_3/SrTiO_3 Mott insulator/band insulator heterointerfaces for various configurations. The (001)-oriented n-type VO_2/LaO/TiO_2 polar discontinuity is conducting, exhibiting a LaVO_3 thickness-dependent metal-insulator transition and low temperature anomalous Hall effect. The (001) p-type VO_2/SrO/TiO_2 interface, formed by inserting a single layer of bulk metallic SrVO_3 or SrO, drives the interface insulating. The (110) heterointerface is also insulating, indicating interface conduction arising from electronic reconstructions.
We report on first principles Self-Interaction Corrected LSD (SIC-LSD) calculations of electronic structure of LaMnO$_{3}$ in the cubic phase. We found a strong tendency to localisation of the Mn $e_{g}$ electron and to orbital ordering. We found the ground state to be orbitally ordered with a staggered order of $x^{2}-z^{2}$ and $y^{2}-z^{2}$ orbits in one plane and this order is repeated along the third direction. The difference in energy with a solution consisting of the ordering of $3x^{2}-r^{2}$ and $3y^{2}-r^{2}$ is, however, very small. The latter ordering is similar to the one observed…
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…
Orientation-driven route to an intrinsic insulating ferromagnetic state in manganite superlattices
Uppsala University（乌普萨拉大学）；Asia Pacific Center for Theoretical Physics（亚太理论物理中心）；King Abdullah University of Science and Technology (KAUST)（阿卜杜拉国王科技大学）；Institute of Physics, Nicolaus Copernicus University（尼古拉·哥白尼大学物理研究所）；School of Physics, Engineering and Technology, University of York（约克大学物理、工程与技术学院）；Department of Physics and Institute of Quantum Convergence and Technology, Kangwon National University（江原国立大学物理系及量子融合技术研究所）；University of Aberdeen（阿伯丁大学）
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 report on the epitaxial strain-driven electronic and antiferromagnetic modulations of a pseudospin-half square lattice realized in superlattices of (SrIrO3)1/(SrTiO3)1. With increasing compressive strain, we find the low-temperature insulating behavior to be strongly suppressed with a corresponding systematic reduction of both the Neel temperature and the staggered moment. However, despite such a suppression, the system remains weakly insulating above the Neel transition. The emergence of metallicity is observed under large compressive strain but only at temperatures far above the Néel tran…
Nominally pure undoped parent manganite LaMnO_3 exhibits a puzzling behavior inconsistent with a simple picture of an A-type antiferromagnetic insulator (A-AFI) with a cooperative Jahn-Teller ordering. We do assign its anomalous properties to charge transfer instabilities and competition between insulating A-AFI phase and metallic-like dynamically disproportionated phase formally separated by a first-order phase transition at T_{disp}=T_{JT}\approx 750 K. The unconventional high-temperature phase is addressed to be a specific electron-hole Bose liquid (EHBL) rather than a simple "chemically" d…
We show that the growth of the heterostructure LaGaO3/SrTiO3 yields the formation of a highly conductive interface. Our samples were carefully analyzed by high resolution electron microscopy, in order to assess their crystal perfection and to evaluate the abruptness of the interface. Their carrier density and sheet resistance are compared to the case of LaAlO3/SrTiO3 and a superconducting transition is found. The results open the route to widening the field of polar-non polar interfaces, pose some phenomenological constrains to their underlying physics and highlight the chance of tailoring the…
First-principles calculations reveal a large cooperative coupling of Jahn-Teller (JT) distortion to oxygen-octahedron rotations in perovskite LaMnO$_3$. The combination of the two distortions is responsible for stabilizing the strongly orthorhombic $A$-AFM insulating ($I$) $Pbnm$ ground state relative to a metallic ferromagnetic (FM-$M$) phase. However, epitaxial strain due to coherent matching to a crystalline substrate can change the relative stability of the two states. In particular, coherent matching to a square-lattice substrate favors the less orthorhombic FM-$M$ phase, with the $A$-AFM…
Decoupling the effects of geometry and nature of strain in LaMnO$_3$: Interplay of dynamic correlations and uniaxial strain driving magnetic phase transitions
Correlated oxides, such as BiMnO$_3$ and LaMnO$_3$, show complex interplay of electronic correlations and crystal structure exhibiting multiple first order phase transitions, some without a clear order parameter. The quantitative theoretical description of this temperature dependent electronic-structural interplay in the vicinity of a Mott transition is still a challenge. Here we address this issue by simultaneously considering both structural and electronic degrees of freedom, within a self-consistent density functional theory with embedded dynamical mean field theory. Our results show the ex…
The latest discovery of possible high temperature superconductivity in the single-layer FeSe film grown on a SrTiO3 substrate, together with the observation of its unique electronic structure and nodeless superconducting gap, has generated much attention. Initial work also found that, while the single-layer FeSe/SrTiO3 film exhibits a clear signature of superconductivity, the double-layer FeSe/SrTiO3 film shows an insulating behavior. Such a dramatic difference between the single-layer and double-layer FeSe/SrTiO3 films is surprising and the underlying origin remains unclear. Here we report ou…
We investigate correlation physics in high-density, two-dimensional electron liquids that reside in narrow SrTiO3 quantum wells. The quantum wells are remotely doped via an interfacial polar discontinuity and the three-dimensional (3D) carrier density is modulated by changing the width of the quantum well. It is shown that even at 3D densities well below one electron per site, short-range Coulomb interactions become apparent in transport, and an insulating state emerges at a critical density. We also discuss the role of disorder in the insulating state.
We employ density functional theory plus dynamical mean field theory and identify the physical origin of why two layers of SrVO$_3$ on a SrTiO$_3$ substrate are insulating: the thin film geometry lifts the orbital degeneracy which in turn triggers a Mott-Hubbard transition. Two layers of SrVO$_3$ are just at the verge of a Mott-Hubbard transition and hence ideally suited for technological applications of the Mott-Hubbard transition: the heterostructure is highly sensitive to strain, electric field, and temperature. A gate voltage can also turn the insulator into a metal, so that a transistor w…
We investigate the electronic properties of the LaAlO3/SrTiO3 interface using density functional theory. In contrast to previous studies, which relied on (semi-)local functionals and the GGA+U method, we here use a recently developed hybrid functional to determine the electronic structure. This approach offers the distinct advantage of accessing both the metallic and insulating multilayers on a parameter-free equal footing. As compared to calculations based on semilocal GGA functionals, our hybrid functional calculations lead to a considerably increased band gap for the insulating systems. The…
Using local density approximation (LDA) calculations we predict GdFeO$_3$-like rotation of TiO$_6$ octahedra at the $n$-type interface between LaAlO$_3$ and SrTiO$_3$. The narrowing of the Ti $d$ bandwidth which results means that for very modest values of $U$, LDA$+U$ calculations predict charge and spin ordering at the interface. Recent experimental evidence for magnetic interface ordering may be understood in terms of the close proximity of an antiferromagnetic insulating ground state to a ferromagnetic metallic excited state.
We investigate the effect of oxygen vacancies and hydrogen dopants at the surface and inside slabs of LaAlO3, SrTiO3, and LaAlO3/SrTiO3 heterostructures on the electronic properties by means of electronic structure calculations as based on density functional theory. Depending on the concentration, the presence of these defects in LaAlO3 slab can suppress the surface conductivity. In contrast, in insulating SrTiO3 slabs already very small concentrations of oxygen vacancies or hydrogen dopant atoms induce a finite occupation of the conduction band. Surface defects in insulating LaAlO3/SrTiO3 het…
The mechanism responsible for the extraordinary interface conductivity of LaAlO$_{3}$ on SrTiO$_{3}$ and its insulator-metal transition remains controversial. Here, using density functional theory calculations, we establish a comprehensive and coherent picture that the interplay of electronic reconstructions, lattice distortions, and surface oxygen vacancies fully compensates the polarization potential divergence in LaAlO$_{3}$/SrTiO$_{3}$, explaining naturally the experimental observations under different conditions. While lattice distortions and a charge redistribution between LaO and AlO$_2…
Despite its simple structure and low degree of electronic correlation, SrTiO$_3$ (STO) features collective phenomena linked to charge transport and, ultimately, superconductivity, that are not yet fully explained. Thus, a better insight in the nature of the quasiparticles shaping the electronic and conduction properties of STO is needed. We studied the low energy excitations of bulk STO and of the LaAlO$_{3}$/SrTiO$_{3}$ two dimensional electron gas (2DEG) by Ti L$_3$ edge resonant inelastic x-ray scattering. In all samples, we find the hallmark of polarons in the form of intense $dd$+phonon e…
Bulk magnetization in Pr_{0.6}Ca_{0.4}MnO_3 thin films with tensile (SrTiO_3) and compressive (LaAlO_3) substrate-induced strain is compared to the magnetooptical Kerr effect (MOKE) measurements. In the absence of an external magnetic field, in both films, a stable ferromagnetic insulating majority phase coexists with an antiferromagnetic insulating phase below ~120K. MOKE measurements indicate that at 5K a metastable ferromagnetic metallic (FM) phase is formed at the surface of the stretched film in a magnetic field below 1.1T already, while in the bulk the FM phase starts to form in the fiel…
We present an ab initio study of the (001) interfaces between two insulating perovskites, the polar LaAlO3 and the nonpolar SrTiO3. We observe an insulating-to-metallic transition above a critical LaAlO3 thickness. We explain that the high conductivity observed at the TiO2 /LaO interface and the lack of similar conductivity at the SrO/AlO2 interface are inherent in the atomic geometry of the system. A large interfacial hopping matrix element between cations causes the formation of a bound electron state at the TiO2 /LaO interface. This mechanism for the formation of interfacial bound states su…
The relative importance of atomic defects and electron transfer in explaining conductivity at the crystalline LaAlO3/SrTiO3 interface has been a topic of debate. Metallic interfaces with similar electronic properties produced by amorphous oxide overlayers on SrTiO3 have called in question the original polarization catastrophe model. We resolve the issue by a comprehensive comparison of (100)-oriented SrTiO3 substrates with crystalline and amorphous overlayers of LaAlO3 of different thicknesses prepared under different oxygen pressures. For both types of overlayers, there is a critical thicknes…
The electro-magnetic properties of ultrathin epitaxial ruthenate films have long been the subject of debate. Here we combine experimental with theoretical investigations of (SrTiO3)5-(SrRuO3)n-(SrTiO3)5 (STO5-SROn-STO5) heterostructures with n = 1 and 2 unit cells, including extensive atomic-resolution scanning-transmission-electron-microscopy imaging, electron-energy-loss-spectroscopy chemical mapping, as well as transport and magneto-transport measurements. The experimental data demonstrate that the STO5-SRO2-STO5 heterostructure is stoichiometric, metallic, and ferromagnetic with TC ~ 128 K…
The electronic properties of the polar interface between insulating oxides is a subject of great current interest. An exciting new development is the observation of robust magnetism at the interface of two non-magnetic materials LaAlO_3 (LAO) and SrTiO_3 (STO). Here we present a microscopic theory for the formation and interaction of local moments, which depends on essential features of the LAO/STO interface. We show that correlation-induced moments arise due to interfacial splitting of orbital degeneracy. We find that gate-tunable Rashba spin-orbit coupling at the interface influences the exc…
Using density functional calculations we have examined the evolution of the electronic structure of SrRuO3 films grown on SrTiO3 substrates as a function of film thickness. At the ultrathin limit of two monolayers (RuO2-terminated surface) the films are found to be at the brink of a spin-state transition which drives the system to an antiferromagnetic and insulating state. Increasing the film thickness to four monolayers, one finds the surprising result that two entirely different solutions coexist. An antiferromagnetic insulating solution coexists with a metallic solution corresponding to an …
The interface between the two insulating oxides SrTiO$_3$ and LaAlO$_3$ gives rise to a two-dimensional electron system with intriguing transport phenomena, including superconductivity, which are controllable by a gate. Previous measurements on the (001) interface have shown that the superconducting critical temperature, the Hall density, and the frequency of quantum oscillations, vary nonmonotonically and in a correlated fashion with the gate voltage. In this paper we experimentally demonstrate that the (111) interface features a qualitatively distinct behavior, in which the frequency of Shub…
