We study the magnetic structure of the (LaMnO$_3$)$_{2n}$/(SrMnO$_3$)$_n$ superlattices from density-functional calculations. In agreement with the experiments, we find that the magnetism changes with the layer thickness `n'. The reason for the different magnetic structures is shown to be the varying potential barrier across the interface, which controls the leakage of the Mn-e$_g$ electrons from the LMO side to the SMO side. This in turn affects the interfacial magnetism via the carrier-mediated Zener double exchange. For n=1 superlattice, the Mn-e$_g$ electrons are more or less spread over the entire lattice, so that the magnetic behavior is similar to the equivalent alloy compound La$_{2/3}$Sr$_{1/3}$MnO$_3$. For larger n, the e$_g$ electron transfer occurs mostly between the two layers adjacent to the interface, thus leaving the magnetism unchanged and bulk-like away from the interface region.
In this Letter, we present investigations of thermal transport in (LaMnO$_3$)$_n$/(SrMnO$_3$)$_n$ superlattices (SLs) with SL periods $Λ=2n$ between $2$ and $12$ unit cells. The analysis of the experimental data clearly reveals a minimum in the thermal conductivity $κ$ at $Λ=6$ u.c. Furthermore, we theoretically estimate the phonon mean free path to be about $3Λ$ in our SLs. These findings clearly show that, in a wide temperature range of $\pm 100\,$K around room temperature, thermal transport in our manganite SLs is coherent. In addition, we demonstrate that antiferromagnetic magnetic orderin…
We conducted lateral force microscopy measurements on seven [LaMnO$_{3}$]$_{m}$/[SrMnO$_{3}$]$_{n}$ superlattices with varied layer thicknesses. We observe that the friction forces and the friction coefficients initially increase with increasing LaMnO3 top layer thickness, followed by saturation when the top layer thickness exceeds a few nanometers. These observations clearly demonstrate that sliding friction is affected by sub-surface material properties to a depth of several nanometers and is not just determined by dynamics in the contact interface. We argue that the sub-surface dissipated e…
The modulation of charge density and spin order in (LaMnO$_3$)$_{2n}$/(SrMnO$_3$)$_n$ ($n$=1-4) superlattices is studied via Monte Carlo simulations of the double-exchange model. G-type antiferromagnetic barriers in the SrMnO$_{3}$ regions with low charge density are found to separate ferromagnetic LaMnO$_{3}$ layers with high charge density. The recently experimentally observed metal-insulator transition with increasing $n$ is reproduced in our studies, and $n=3$ is found to be the critical value.
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…
We study how strain affects orbital ordering and magnetism at the interface between SrMnO$_3$ and LaMnO$_3$ from density-functional calculations and interpret the basic results in terms of a three-site Mn-O-Mn model. Magnetic interaction between the Mn atoms is governed by a competition between the antiferromagnetic superexchange of the Mn t$_{2g}$ core spins and the ferromagnetic double exchange of the itinerant e$_g$ electrons. While the core electrons are relatively unaffected by the strain, the orbital character of the itinerant electron is strongly affected, which in turn causes a large c…
We report on the electronic properties of superlattices composed of three different antiferromagnetic insulators, NdMnO3/SrMnO3/LaMnO3 grown on SrTiO3 substrates. Photoemission spectra obtained by tuning the x-ray energy at the Mn 2p -> 3d edge show a Fermi cut-off, indicating metallic behavior mainly originating from Mn e_g electrons. Furthermore, the density of states near the Fermi energy and the magnetization obey a similar temperature dependence, suggesting a correlation between the spin and charge degrees of freedom at the interfaces of these oxides.
Polarized neutron reflectivity measurements of a ferromagnetic [(LaMnO$_3$)$_{11.8}$/(SrMnO$_3$)$_{4.4}$]$_6$ superlattice reveal a modulated magnetic structure with an enhanced magnetization at the interfaces where LaMnO$_3$ was deposited on SrMnO$_3$ (LMO/SMO). However, the opposite interfaces (SMO/LMO) are found to have a reduced ferromagnetic moment. The magnetic asymmetry arises from the difference in lateral structural roughness of the two interfaces observed via electron microscopy, with strong ferromagnetism present at the interfaces that are atomically smooth over tens of nanometers. …
Photoinduced magnetization dynamics is investigated in chemically ordered $(\mathrm{LaMnO}_3)_{2n}/(\mathrm{SrMnO}_3)_n$ superlattices using the time-resolved magneto-optic Kerr effect. A monotonic frequency-field dependence is observed for the $n=1$ superlattice, indicating a single spin population consistent with a homogeneous hole distribution. In contrast, for $n\geq2$ superlattices, a large precession frequency is observed at low fields indicating the presence of an exchange torque in the dynamic regime. We propose a model that ascribes the emergence of exchange torque to the coupling bet…
We use resonant soft x-ray scattering to study electronic reconstruction at the interface between the Mott insulator LaMnO3 and the "band" insulator SrMnO3. Superlattices of these two insulators were shown previously to have both ferromagnetism and metallic tendencies [Koida et al., Phys. Rev. B 66, 144418 (2002)]. By studying a judiciously chosen superlattice reflection we show that the interface density of states exhibits a pronounced peak at the Fermi level, similar to that predicted by Okamoto et al. [Phys. Rev. B 70, 241104(R) (2004)]. The intensity of this peak correlates with the conduc…
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…
We have studied the influence of epitaxial strain on magnetic orderings and the couplings between the spin and polar phonons in the 1:1 SrMnO$_3$/LaMnO$_3$ superlattice from first principles. Magnetic phase transitions of the superlattice induced by epitaxial strain are observed, consistent with previous reports. We find that oxygen octahedral rotations lower the ground state energy but do not destroy the magnetic phase transitions induced by strain. We compute zone center phonon frequencies and eigenvectors as functions of epitaxial strain and magnetic ordering. A substantial increase of the …
Electronic reconstruction at the polar interface LaMnO$_3$/SrMnO$_3$ (LMO/SMO) (100) resulting from the polar catastrophe is studied from a model Hamiltonian that includes the double and super exchange interactions, the Madelung potential, and the Jahn-Teller coupling terms relevant for the manganites. We show that the polar catastrophe, originating from the alternately charged LMO layers and neutral SMO layers, is quenched by the accumulation of an extra half electron per cell in the interface region as in the case of the LaAlO$_3$/SrTiO$_3$ interface. In addition, the Mn e$_g$ electrons leak…
Exchange interactions and finite-temperature magnetism in (111)-oriented (LaMnO$_3$)$_{2n}$|(SrMnO$_3$)$_n$ superlattices
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）；Department of Energy Technology, Korea Institute of Energy Technology (KENTECH)（韩国能源技术研究院能源技术部）；Department of Physics and Astronomy, Uppsala University（乌普萨拉大学物理与天文系）
Motivated by recent experiments, we use the $+U$ extension of the generalized gradient approximation to density functional theory to study superlattices composed of alternating layers of LaNiO$_3$ and LaMnO$_3$. For comparison we also study a rocksalt ((111) double perovskite) structure and bulk LaNiO$_3$ and LaMnO$_3$. A Wannier function analysis indicates that band parameters are transferable from bulk to superlattice situations with the exception of the transition metal d-level energy, which has a contribution from the change in d-shell occupancy. The charge transfer from Mn to Ni is found …
Taking advantage of the large electron escape depth of soft x-ray angle resolved photoemission spectroscopy we report electronic structure measurements of (111)-oriented [LaNiO3/LaMnO3] superlattices and LaNiO3 epitaxial films. For thin films we observe a 3D Fermi surface with an electron pocket at the Brillouin zone center and hole pockets at the zone vertices. Superlattices with thick nickelate layers present a similar electronic structure. However, as the thickness of the LaNiO3 is reduced the superlattices become insulating. These heterostructures do not show a marked redistribution of spe…
Oxygen octahedral rotations have been measured in short-period (LaNiO$_3$)$_n$/(SrMnO$_3$)$_m$ superlattices using synchrotron diffraction. The in-plane and out-of-plane bond angles and lengths are found to systematically vary with superlattice composition. Rotations are suppressed in structures with $m>n$, producing a nearly cubic form of LaNiO$_3$. Large rotations are present in structures with $m<n$, leading to reduced bond angles in SrMnO$_3$. The metal-oxygen-metal bond lengths decrease as rotations are reduced, in contrast to behavior previously observed in strained, single layer films. …
The exchange coupling at the interfaces of magnetic superlattices consisting of ferromagnetic $SrRuO_3$ and antiferromagnetic $SrMnO_3$ grown on (001) oriented $SrTiO_3$ is studied with in-plane and out-of-plane orientations, with respect to the substrate plane, of the cooling magnetic field. The magnetization of the in-plane, field cooled hysteresis loop is lower than the corresponding in-plane zero-field-cooled hysteresis loop. The out-of-plane field cooled hysteresis loop is shifted, from the origin, along the graphical magnetization axis. We attribute this irreversible rotation of the mome…
Strain-induced structural transitions in (111)-oriented (LaMnO$_3$)$_{2n}|$(SrMnO$_3$)$_n$ superlattices
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, School of Natural and Computing Sciences, University of Aberdeen（阿伯丁大学自然与计算科学学院物理系）；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）；Department of Physics and Astronomy, Uppsala University（乌普萨拉大学物理与天文学系）
Charge transfer in superlattices consisting of SrIrO$_3$ and SrMnO$_3$ is investigated using density functional theory. Despite the nearly identical work function and non-polar interfaces between SrIrO$_3$ and SrMnO$_3$, rather large charge transfer was experimentally reported at the interface between them. Here, we report a microscopic model that captures the mechanism behind this phenomenon, providing a qualitative understanding of the experimental observation. This leads to unique strain dependence of such charge transfer in iridate-manganite superlattices. The predicted behavior is consist…
(LaNiO3)n/(LaMnO3)2 superlattices were grown using ozone-assisted molecular beam epitaxy, where LaNiO3 is a paramagnetic metal and LaMnO3 is an antiferromagnetic insulator. The superlattices exhibit excellent crystallinity and interfacial roughness of less than 1 unit cell. X-ray spectroscopy and dichroism measurements indicate that electrons are transferred from the LaMnO3 to the LaNiO3, inducing magnetism in LaNiO3. Magnetotransport measurements reveal a transition from metallic to insulating behavior as the LaNiO3 layer thickness is reduced from 5 unit cells to 2 unit cells and suggest a mo…
We investigated the magnetic and optical properties of [(LaMnO3)n/(SrTiO3)8]20 (n = 1, 2, and 8) superlattices grown by pulsed laser deposition. We found a weak ferromagnetic and semiconducting state developed in all superlattices. An analysis of the optical conductivity showed that the LaMnO3 layers in the superlattices were slightly doped. The amount of doping was almost identical regardless of the LaMnO3 layer thickness up to eight unit cells, suggesting that the effect is not limited to the interface. On the other hand, the magnetic ordering became less stable as the LaMnO3 layer thickness…
A direct correlation is seen between the coercive field (HC) and the magnetic-field-dependent resistivity (MR) in SrMnO3/SrRuO3 superlattices of perpendicular magnetic anisotropy. The magnetoresistance shows a sharp jump at Hc for in-plane current and the out-of-plane magnetic field. Both HC and high-field MR also oscillate with the thickness of the SrMnO3 spacer layers separating the metallic ruthenate. Since the spacer in these superlattices has no mobile carriers to facilitate an oscillatory coupling, we attribute the observed behavior to the spin-polarized quantum tunneling of electrons be…
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…
The emergence of magnetic reconstructions at the interfaces of oxide heterostructures are often explained via subtle modifications in the electronic densities, exchange couplings, or strain. Here an additional possible route for induced magnetism is studied in the context of the (LaNiO$_3$)$_n$/(LaMnO$_3$)$_n$ superlattices using a hybrid tight-binding model. In the LaNiO$_3$ region, the induced magnetizations decouple from the intensity of charge leakage from Mn to Ni, but originate from the spin-filtered quantum confinement present in these nanostructures. In general, the induced magnetizati…
Insulating band gaps both below and above the Néel temperature in d-electron LaTiO3, LaVO3, SrMnO3, and LaMnO3 perovskites as a symmetry-breaking event
In a recent publication (S. Dong et al., Phys. Rev. Lett.103, 127201 (2009)), two (related) mechanisms were proposed to understand the intrinsic exchange bias present in oxides heterostructures involving G-type antiferromagnetic perovskites. The first mechanism is driven by the Dzyaloshinskii-Moriya interaction, which is a spin-orbit coupling effect. The second is induced by the ferroelectric polarization, and it is only active in heterostructures involving multiferroics. Using the SrRuO$_3$/SrMnO$_3$ superlattice as a model system, density-functional calculations are here performed to verify …
The functional properties of transition metal perovskite oxides are known to result from a complex interplay of magnetism, polarization, strain, and stoichiometry. Here, we show that for materials with a cooperative Jahn-Teller distortion, such as LaMnO$_3$ (LMO), the orbital order can also couple to the defect chemistry and induce novel material properties. At low temperatures, LMO exhibits a strong Jahn-Teller distortion that splits the $e_g$ orbitals of the high-spin Mn$^{3+}$ ions and leads to alternating long, short, and intermediate Mn--O bonds. Our DFT+$U$ calculations show that, as a r…
By means of ab initio calculations the possibilities of switchable spin-polarized two-dimensional electron gas (2DEG) at the interface of antiferromagnetic and ferroelectric perovskites, i.e., LaMnO3/BaTiO3 superlattice, were investigated. We demonstrate that at the heterostructure with TiO2/LaO interfacial layers the two-dimensional conducting state arises mainly localized within the interfacial MnO layer. The density of states at the Fermi-level can be tuned by ferroelectric polarization reversal. The conducting state coexists with magnetic one mainly arose from Mn atoms.
Heterostructures of mixed-valence manganites are still under intense scrutiny, due to the occurrence of exotic quantum phenomena linked to electronic correlation and interfacial composition. For instance, if two anti-ferromagnetic insulators as LaMnO$_3$ and SrMnO$_3$ are grown in a (001)-oriented superlattice, a half-metallic ferromagnet may form, provided that the thickness is sufficiently small to allow tunneling across interfaces. In this article, we employ electronic structure calculations to show that all the layers of a (111)-oriented LaMnO$_3$|SrMnO$_3$ superlattice retain a half-metal…
Modulation-doped oxide two-dimensional electron gas (2DEG) formed at the LaMnO3 (LMO) buffered disorderd-LaAlO3/SrTiO3 (d-LAO/LMO/STO) heterointerface, provides new opportunities for electronics as well as quantum physics. Herein, we studied the dependence of Sr-doping of La1-xSrxMnO3 (LSMO, x=0, 1/8, 1/3, 1/2, and 1) thus the filling of the Mn eg subbands as well as the LSMO polarity on the transport properties of d-LAO/LSMO/STO. Upon increasing the LSMO film thickness from 1 unit cell (uc) to 2 uc, a sharp metal to insulator transition of interface conduction was observed, independent of x. …
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…
Controlling the electronic properties of interfaces has enormous scientific and technological implications and has been recently extended from semiconductors to complex oxides which host emergent ground states not present in the parent materials. These oxide interfaces present a fundamentally new opportunity where, instead of conventional bandgap engineering, the electronic and magnetic properties can be optimized by engineering quantum many-body interactions. We utilize an integrated oxide molecular-beam epitaxy and angle-resolved photoemission spectroscopy system to synthesize and investigat…
The formation of a novel spin-polarized 2D electron gas at the LaMnO$_3$ monolayer embedded in SrMnO$_3$ is predicted from the first-principles density-functional calculations. The La (d) electrons become confined in the direction normal to the interface in the potential well of the La layer, serving as a positively-charged layer of electron donors. These electrons mediate a ferromagnetic alignment of the Mn t$_{2g}$ spins near the interface via the Anderson-Hasegawa double exchange and become, in turn, spin-polarized due to the internal magnetic fields of the Mn moments.
We report the \QTR{it}{pinned/biased} \QTR{it}{moment} in the superlattices consisting of ferromagnetic (FM) SrRuO$_3$ and antiferromgnetic (AFM) SrMnO$_3$. This superlattice system shows anisotropy and oriented pinning/biasing in the field-cooled (FC) hysteresis loop. The in-plane cooling-field provides antiferromagnetic orientations while out-of-plane cooling-field provides ferromagnetic orientations to the pinned/biased moments. The spacer layer thickness, strength and orientation of magnetic field, cooling field, and driving current influence the pinning strength. We propose that the magne…
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…
We have observed the pinned/biased moments in the superlattices consisting of ferromagnetic (FM) SrRuO3 (SRO) and antiferromagnetic (AFM) SrMnO3 (SMO)bilayer. The alternate stacking of SRO and SMO leading to a low field positive magnetoresistance with enhanced hysteretic field dependent magnetoresistance under the application of the out-of-plane magnetic field. We attribute these effects to the observed biased/pinned magnetic moments in the SRO layer in the vicinity of the interfaces. In addition, the biased/pinned moments can be oriented under the application of either the out-of-plane magnet…
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 present experimental and theoretical investigations of phonon thermal transport in (LaMnO$_3$)$_m$/(SrMnO$_3$)$_n$ superlattices (LMO/SMO SLs) with the thickness of individual layers $m,n = 3 - 10\;$ u.c. and the thickness ratio $m/n = 1, 2$. Optical transient thermal reflectivity measurements reveal a pronounced difference in the thermal conductivity between SLs with $m/n = 1$, and SLs with $m/n = 2$. State-of-the art electron microscopy techniques and ab-initio density functional calculations enables us to assign the origin of this difference to the absence ($m/n = 1$) or presence ($m/n =…
We report a modulation of the in-plane magnetotransport in artificial manganite superlattice (SL) [(NdMnO3)n /(SrMnO3)n /(LaMnO3)n]m by varying the layer thickness n while keeping the total thickness of the structure constant. Charge transport in these heterostructures is confined to the interfaces and occurs via variable range hopping (VRH). Upon increasing n, the interfacial separation rises, leading to a suppression of the electrostatic screening between carriers of neighboring interfaces and the opening of a Coulomb gap at the Fermi level (EF). The high-field magnetoresistance (MR) is univ…
Heterostructured material systems devoid of ferroic components are presumed not to display ordering associated with ferroelectricity. In heterostructures composed of transition metal oxides, however, the disruption introduced by an interface can affect the balance of the competing interactions among electronic spins, charges and orbitals. This has led to the emergence of properties absent in the original building blocks of a heterostructure, including metallicity, magnetism and superconductivity. Here we report the discovery of ferroelectricity in artificial tri-layer superlattices consisting …
