We investigate the electronic reconstruction at the interface between ferromagnetic metallic (FM) and antiferromagnetic insulating (AFI) manganites in superlattices using a two-orbital double-exchange model including superexchange interactions, Jahn-Teller lattice distortions, and long range Coulomb interactions. The magnetic and the transport properties critically depend on the thickness of the AFI layers. We focus on superlattices where the constituent parent manganites have the same electron density n = 0.6. The induced ferromagnetic moment in the AFI layers decreases monotonically with increasing layer width, and the electron-density profile and the magnetic structure in the center of the AFI layer gradually return to the bulk limit. The width of the AFI layers and the charge-transfer profile at the interfaces control the magnitude of the magnetoresistance and the metal-insulator transition of the FM/AFI superlattices.
We use a two-orbital double-exchange model including Jahn-Teller lattice distortions, superexchange interactions, and long-range Coulomb (LRC) interactions to investigate the origin of magnetically disordered interfaces between ferromagnetic metallic (FM) and antiferromagnetic insulating (AFI) manganites in FM/AFI superlattices. The induced magnetic moment in the AFI layer varies non-monotonically with increasing AFI layer width as seen in the experiment. We provide a framework for understanding this non-monotonic behavior which has a one-to-one correspondence with the magnetization of the FM …
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…
A theoretical model is proposed for the (0,0,1) superlattice manganite system (LaMnO$_3$)$_n$(SrMnO$_3$)$_m$. The model includes the electron-electron, electron-phonon, and cooperative Jahn-Teller interactions. It is solved using a version of single-site the dynamical mean field approximation generalized to incorporate the cooperative Jahn-Teller effect. The phase diagram and conductivities are calculated. The behavior of the superlattice is found to a good approximation to be an average over the density-dependent properties of individual layers, with the density of each layer fixed by electro…
We demonstrate that delta-doping can be used to create a dimensionally confined region of metallic ferromagnetism in an antiferromagnetic (AF) manganite host, without introducing any explicit disorder due to dopants or frustration of spins. Delta-doped carriers are inserted into a manganite superlattice (SL) by a digital-synthesis technique. Theoretical consideration of these additional carriers show that they cause a local enhancement of ferromagnetic (F) double-exchange with respect to AF superexchange, resulting in local canting of the AF spins. This leads to a highly modulated magnetizatio…
The nature of the magnetic order in (La2/3Sr1/3MnO3)9/(LaNiO3)3 superlattices is investigated using x-ray resonant magnetic reflectometry. We observe a new c-axis magnetic helix state in the (LaNiO3)3 layers that had never been reported in nickelates, and which mediates the ~130deg magnetic coupling between the ferromagnetic (La2/3Sr1/3MnO3)9 layers, illustrating the power of x-rays for discovering the magnetic state of complex oxide interfaces. Resonant inelastic x-ray scattering and x-ray absorption spectroscopy show that Ni-O ligand hole states from bulk LaNiO3 are mostly filled due to inte…
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…
(Pr,Ca)MnO3 is the archetypal charge-ordered manganite, but in Pr0.48Ca0.52MnO3 we find (using convergent-beam electron diffraction and dark-field images) that the superlattice period is locally incommensurate with respect to the parent lattice, and that the superlattice orientation possesses significant local variations. This suggests that local electron-lattice coupling never overwhelmingly dominates the rich physics of manganites, even in the most extreme scenarios that produce the largest colossal magnetoresistance effects.
We use femtosecond x-ray diffraction to study the structural response of charge and orbitally ordered Pr$_{1-x}$Ca$_x$MnO$_3$ thin films across a phase transition induced by 800 nm laser pulses. By investigating the dynamics of both superlattice reflections and regular Bragg peaks, we disentangle the different structural contributions and analyze their relevant time-scales. The dynamics of the structural and charge order response are qualitatively different when excited above and below a critical fluence $f_c$. For excitations below $f_c$ the charge order and the superlattice is only partially…
In addition to mechanisms already proposed to account for the formation in manganites of a small-polaron superlattice above the Curie temperature Tc and to a metallic-like sea of large polarons below Tc, we now consider other observed colossal-resistance inducing fields, such as magnetic, electric, photon, or strain fields. We attribute the charge-ordered phase formation to the occurrence of strong dipolar binding of vibronic small polarons arising from the phonon coupling of highly polarizable two-level orbital systems. These species having associated inherent electric and magnetic off-center…
We explore manganite interface magnetism in epitaxially grown La0.7Sr0.3MnO3(LSMO)/SrTiO3 ultrathin superlattices (SL) along (110) orientation. we show that robust ferromagnetism persists down to four monolayers LSMO(MLs) (~1.1 nm in thickness), of which 50% Mn is at the interface state. Above eight MLs, the magnetic moment is nearly saturated to the theoretical value of 3.7u_B, with an estimated interface moment of 3.2u_B. In comparison to (100)-oriented SLs which were previously shown to have a spin canted ground state, (110)-oriented SLs exhibit stronger low-dimensional ferromagnetism and b…
We report on a resonant soft X-ray spectroscopy study of the electronic and magnetic structure of the cuprate-manganite interface. Polarized X-ray spectroscopy measurements taken at the Cu L edge reveal up to a five-fold increase in the dichroic signal as compared to past experimental and theoretical values. Furthermore an increase in the degree of interlayer charge transfer up to 0.25e (where e is charge of an electron) per copper ion is observed leading to a profound reconstruction in the orbital scheme for these interfacial copper ions. It is inferred that these enhancement are related to a…
An oxide heterostructure made of manganite bilayers and ferroelectric perovskites is predicted to lead to the full control of magnetism when switching the ferroelectric polarizations. By using asymmetric polar interfaces in the superlattices, more electrons occupy the Mn layer at the $n$-type interface side than at the $p$-type side. This charge disproportionation can be enhanced or suppressed by the ferroelectric polarization. Quantum model and density functional theory calculations reach the same conclusion: a ferromagnetic-ferrimagnetic phase transition with maximal change $>90%$ of the tot…
The self-organization of strongly interacting electrons into superlattice structures underlies the properties of many quantum materials. How these electrons arrange within the superlattice dictates what symmetries are broken and what ground states are stabilized. Here we show that cryogenic scanning transmission electron microscopy enables direct mapping of local symmetries and order at the intra-unit-cell level in the model charge-ordered system Nd$_{1/2}$Sr$_{1/2}$MnO$_{3}$. In addition to imaging the prototypical site-centered charge order, we discover the nanoscale coexistence of an exotic…
The magnetic nature of the B-site dopants controls the magnetic phases in B-site doped manganites RE$_{1-x}$AE$_{x}$Mn$_{1-η}$B$_η$O$_3$. Different B-site dopants of equal valence, doped into the same reference manganite, lead to different magnetic phases at low temperature, which can not be explained using the valence change scenario. We focus on trivalent B-site dopants in CE-CO-OO-I manganites at half-filling $x=0.50$ to study the role of magnetic interactions between the B-site dopants and the neighboring Mn-sites by using a two-orbital double-exchange model including super-exchange intera…
Here we report about the interface reconstruction in the recently discovered superconducting artificial superlattices based on insulating CaCuO2 and SrTiO3 blocks. Hard x-ray photoelectron spectroscopy shows that the valence bands alignment prevents any electronic reconstruction by direct charge transfer between the two blocks. We demonstrate that the electrostatic built-in potential is suppressed by oxygen redistribution in the alkaline earth interface planes. By using highly oxidizing growth conditions, the oxygen coordination in the reconstructed interfaces may be increased, resulting in th…
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…
The crystalline structure, anisotropic magnetoresistance (AMR), and magnetization of La0.7Sr0.3MnO3/SrTiO3 (LSMO/STO) superlattices grown by an rf sputtering system are systematically analyzed to study the spin polarization of manganite at interfaces. A perfectly epitaxial growth with sharp interfaces between LSMO and STO layers is confirmed by the transmission electron microscopy (TEM) image and the x-ray diffraction. The presence of positive low-temperature AMR in LSMO/STO superlattices with thinner LSMO layers or thicker STO layers implies that two bands of majority and minority character c…
Scalar spin chirality is expected to induce a finite contribution to the Hall response at low temperatures. We study this spin-chirality-driven Hall effect, known as the topological Hall effect, at the manganite side of the interface between La$_{1-x}$Sr$_{x}$MnO$_{3}$ and SrIrO$_3$. The ferromagnetic double-exchange hopping at the manganite layer, in conjunction with the Dzyaloshinskii-Moriya (DM) interaction which arises at the interface due to broken inversion symmetry and strong spin-orbit coupling from the iridate layer, could produce a skyrmion-crystal (SkX) phase in the presence of an e…
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）
We have recently argued that manganites do not possess stripes of charge order, implying that the electron-lattice coupling is weak [Phys Rev Lett \textbf{94} (2005) 097202]. Here we independently argue the same conclusion based on transmission electron microscopy measurements of a nanopatterned epitaxial film of La$_{0.5}$Ca$_{0.5}$MnO$_3$. In strain relaxed regions, the superlattice period is modified by 2-3% with respect to the parent lattice, suggesting that the two are not strongly tied.
An interface modification of LCMO-BTO superlattices was found to massively influence magnetic and magnetotransport properties. Moreover it determines the crystal structure of the manganite layers, changing it from orthorhombic (Pnma) for the conventional superlattice (cSL), to rhombohedral (R-3c) for the modified one (mSL). While the cSL shows extremely nonlinear ac transport, the mSL is an electrically homogeneous material. The observations go beyond an oversimplified picture of dead interface layers and evidence the importance of electronic correlations at perovskite interfaces.
The recently discovered structural reconstruction in the cuprate superlattice (SrCuO$_2$)$_n$/(SrTiO$_3$)$_2$ has been investigated across the critical value of $n=5$ using resonant inelastic x-ray scattering (RIXS). We find that at the critical value of $n$, the cuprate layer remains largely in the bulk-like two-dimensional structure with a minority of Cu plaquettes being reconstructed. The partial reconstruction leads to quenching of the magnons starting at the $Γ$-point due to the minority plaquettes acting as scattering points. Although comparable in relative abundance, the doped charge im…
The interfacial properties of Y0.6Pr0.4Ba2Cu3O7/La2/3Ca1/3MnO3 superlattices have been studied by resonant soft x-rays and diffuse scattered neutrons. Linearly polarized X-ray absorption at Cu L3 -edge reveals dramatic interfacial changes from the bulk including charge transfer between LCMO and YPBCO and an orbital reconstruction in the interface CuO2 plane. The similarities to the case of zero Pr-doping are due to the strongly hybridized covalent bond between Cu and Mn. However, reduced charge transfer and a more bulk-like interfacial orbital occupation are observed and related to the effect …
We perform density functional theory plus dynamical mean field theory calculations to investi- gate internal charge transfer in an artificial superlattice composed of alternating layers of vanadate and manganite perovskite and Ruddlesden-Popper structure materials. We show that the elec- tronegativity difference between vanadium and manganese causes moderate charge transfer from VO2 to MnO2 layers in both perovskite and Ruddlesden-Popper based superlattices, leading to hole doping of the VO2 layer and electron doping of the MnO2 layer. Comparison of the perovskite and Ruddlesden-Popper based h…
Magnetic structures and the relationship between spin and charge-orbital orderings of an A-site ordered double-perovskite manganite SmBaMn2O6, an anticipated multiferroic material, were investigated by means of neutron diffraction. The spin arrangement in MnO2 planes perpendicular to the c axis is revealed to be the same as that in the A-site disordered half-doped manganites CE-type but the stacking pattern is found to be different displaying a unique twofold period. The temperature dependence of the superlattice magnetic and nuclear reflections clarifies that the antiferromagnetic spin orderi…
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.
Polarized Neutron Reflectometry and magnetometry measurements have been used to obtain a comprehensive picture of the magnetic structure of a series of La{2/3}Sr{1/3}MnO{3}/Pr{2/3}Ca{1/3}MnO{3} (LSMO/PCMO) superlattices, with varying thickness of the antiferromagnetic (AFM) PCMO layers (0<=t_A<=7.6 nm). While LSMO presents a few magnetically frustrated monolayers at the interfaces with PCMO, in the latter a magnetic contribution due to FM inclusions within the AFM matrix was found to be maximized at t_A~3 nm. This enhancement of the FM moment occurs at the matching between layer thickness and …
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 epitaxial stabilization of a single layer or superlattice structures composed of complex oxide materials on polar (111) surfaces is severely burdened by reconstructions at the interface, that commonly arise to neutralize the polarity. We report on the synthesis of high quality LaNiO$_3$/mLaAlO$_3$ pseudo cubic (111) superlattices on polar (111)-oriented LaAlO$_3$, the proposed complex oxide candidate for a topological insulating behavior. Comprehensive X-Ray diffraction measurements, RHEED, and element specific resonant X-ray absorption spectroscopy affirm their high structural and chemica…
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…
We study the effect of uniform uniaxial strain on the ground state electronic configuration of a thin film manganite. Our model Hamiltonian includes the double-exchange, the Jahn-Teller electron-lattice coupling, and the antiferromagnetic superexchange. The strain arises due to the lattice mismatch between an insulating substrate and a manganite which produces a tetragonal distortion. This is included in the model via a modification of the hopping amplitude and the introduction of an energy splitting between the Mn e_g levels. We analyze the bulk properties of half-doped manganites and the ele…
The ferromagnetic and insulating state observed in La$_{1-x}$Ca$_{x}$MnO$_3$, 0.125$<$x$<$0.2, is characterized by structural and magnetic anomalies below T$_C$, similar to those observed in the x$_{Sr}$$\approx$1/8. A neutron scattering study of the superlattice {\bf Q$_0$}= (0,0,1+/4)$_{cub}$ peak, and of the magnetic excitations are reported in the x$_{Ca}$=0.2 sample. The occurrence of this superstructure is associated with the observation of a gap in the spin dynamics, at a {\bf q$_0$} wave-vector ({\bf q$_0$}={\bf Q$_0$}-$τ$) with the same modulus $|${\bf q$_0$}$|$ in all directions, whi…
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…
We report an investigation of the combined structural and electronic properties of the bronze Na$_{1.5}$(PO$_{2}$)$_{4}$(WO$_{3}$)$_{20}$. Its low dimensional structure and possible large reconstruction of the Fermi surface due to charge density wave instability makes this bulk material a natural superlattice with a reduced number of carriers and Fermi energy. Signatures of multilayered 2D electron weak localization are consequently reported, with an enhanced influence of quantum oscillations. A crossover between these two antagonistic entities previously observed only in genuine low dimension…
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…
We have measured photoemission spectra of SrTiO3/LaTiO3 superlattices with a topmost SrTiO3 layer of variable thickness. Finite coherent spectral weight with a clear Fermi cut-off was observed at chemically abrupt SrTiO3/LaTiO3 interfaces, indicating that an ``electronic reconstruction'' occurs at the interface between the Mott insulator LaTiO3 and the band insulator SrTiO3. For SrTiO3/LaTiO3 interfaces annealed at high temperatures (~ 1000 C), which leads to Sr/La atomic interdiffusion and hence to the formation of La1-xSrxTiO3-like material, the intensity of the incoherent part was found to …
The experimental observation that vanadate superlattices (LaVO$_3$)$_m$/SrVO$_3$ show ferromagnetism up to room temperature [U.\ Lüders {\it et al.}, Phys.\ Rev.\ B {\bf 80}, 241102R (2009)] is investigated by means of density functional theory. First, the influence of the density functional on the electronic and magnetic structure of bulk ${\rm LaVO_3}$ is discussed. Second, the band structure of a (LaVO$_3$)$_m$/SrVO$_3$ slab for $m=5$ and 6 is calculated. Very different behaviors for odd and even values of $m$ are found: In the odd case lattice relaxation results into a buckling of the inte…
The electronic symmetry of the SrTiO3/LaAlO3 interface was investigated by optical second harmonic generation, using superlattices with varying periodicity to study the evolution of the electronic reconstruction while avoiding substrate contributions. The superlattices show large perpendicular optical nonlinearity, which abruptly increases when the sublattice thickness goes above 3 unit cells, revealing substantial effects of the polar-nonpolar interface. The nonlinear 'active' area is primarily in SrTiO3, develops with increasing thickness, and extends up to 8 unit cells from the interface.
We examine the anomalous inverse spin switch behavior in La$_{0.7}$Ca$_{0.3}$MnO$_3$ (LCMO)/YBa$_2$Cu$_3$O$_{7-δ}$ (YBCO)/LCMO trilayers by combined transport studies and polarized neutron reflectometry. Measuring magnetization profiles and magnetoresistance in an in-plane rotating magnetic field, we prove that, contrary to many accepted theoretical scenarios, the relative orientation between the two LCMO's magnetizations is not sufficient to determine the magnetoresistance. Rather the field dependence of magnetoresistance is explained by the interplay between the applied magnetic field and th…
With x-ray absorption spectroscopy we investigated the orbital reconstruction and the induced ferromagnetic moment of the interfacial Cu atoms in YBa$_2$Cu$_3$O$_{7}$/La$_{2/3}$Ca$_{1/3}$MnO$_3$ (YBCO/LCMO) and La$_{2-x}$Sr$_{x}$CuO$_4$/La$_{2/3}$Ca$_{1/3}$MnO$_3$ (LSCO/LCMO) multilayers. We demonstrate that these electronic and magnetic proximity effects are coupled and are common to these cuprate/manganite multilayers. Moreover, we show that they are closely linked to a specific interface termination with a direct Cu-O-Mn bond. We furthermore show that the intrinsic hole doping of the cuprat…
The interplay of nearly degenerate orders in quantum materials can lead to a myriad of emergent phases. A prominent case is that of the high-Tc cuprates for which the relationship between superconductivity and a short-ranged, incommensurate charge density wave in the CuO2 planes involving the dx2-y2 orbitals (Cu-CDW) is a subject of great current interest. Strong modifications of the strength and coherence of this Cu-CDW have been achieved by applying large magnetic fields, uniaxial pressure, or via the interfacial coupling in cuprate/manganite multilayers. However, such modifications do not a…
We investigate the electronic reconstruction in (LaNiO$_{3}$)$_n$/(LaAlO$_{3}$)$_3$ (n=3, 5 and 10) superlattices due to the quantum confinement (QC) by d.c. transport and resonant soft x-ray absorption spectroscopy. In proximity to the QC limit, a Mott-type transition from an itinerant electron behavior to a localized state is observed. The system exhibits tendency towards charge-order during the transition. ab initio cluster calculations are in good agreement with the absorption spectra, indicating that the apical ligand hole density is highly suppressed resulting in a strong modification of…
We report measurements of the thermoelectric power and electrical resistivity of superlattices composed of the high-temperature superconductor YBa2Cu3O(7-delta) (YBCO) and the metallic ferromagnet La(2/3)Ca(1/3)MnO3 (LCMO) with individual layer thicknesses between 5 and 50 nm. Whereas YBCO and LCMO reference films prepared under the same conditions exhibit negative Seebeck coefficients, in excellent agreement with data on bulk compounds of identical composition, those of all superlattices are positive, regardless of the individual layer thickness. Having ruled out lattice strain and incomplete…
Superlattice potentials are theoretically predicted to modify the single-particle electronic structures. The resulting Coulomb-interaction-dominated low-energy physics would generate highly novel many-body phenomena. Here, by in situ tunneling spectroscopy, we show the signatures of superstructure-modulated correlated electron states in epitaxial bilayer graphene (BLG) on 6H-SiC(0001). As the carrier density is locally quasi-'tuned' by the superlattice potentials of a 6x6 interface reconstruction phase, the spectral-weight transfer occurs between the two broad peaks flanking the charge-neutral…
At interfaces between oxide materials, lattice and electronic reconstructions always play important roles in exotic phenomena. In this study, the density functional theory and maximally localized Wannier functions are employed to investigate the (LaTiO$_3$)$_n$/(LaVO$_3$)$_n$ magnetic superlattices. The electron transfer from Ti$^{3+}$ to V$^{3+}$ is predicted, which violates the intuitive band alignment based on the electronic structures of LaTiO$_3$ and LaVO$_3$. Such unconventional charge transfer quenches the magnetism of LaTiO$_3$ layer mostly and leads to metal-insulator transition in th…
The electron-phonon interaction is of central importance for the electrical and thermal properties of solids, and its influence on superconductivity, colossal magnetoresistance, and other many-body phenomena in correlated-electron materials is currently the subject of intense research. However, the non-local nature of the interactions between valence electrons and lattice ions, often compounded by a plethora of vibrational modes, present formidable challenges for attempts to experimentally control and theoretically describe the physical properties of complex materials. Here we report a Raman s…
The combination of charge and spin degrees of freedom with electronic correlations in condensed matter systems leads to a rich array of phenomena, such as magnetism, superconductivity, and novel conduction mechanisms. While such phenomena are observed in bulk materials, a richer array of behaviors becomes possible when these degrees of freedom are controlled in atomically layered heterostructures, where one can constrain dimensionality and impose interfacial boundary conditions. Here, we unlock a host of unique, hidden electronic and magnetic phase transitions in NdNiO$_3$ while approaching th…
Charge transfer in oxide heterostructures can be tuned to promote emergent interfacial states, and accordingly, has been the subject of intense study in recent years. However, accessing the physics at these interfaces, which are often buried deep below the sample surface, remains difficult. Addressing this challenge requires techniques capable of measuring the local electronic structure with high-resolution depth dependence. Here, we have used linearly-polarized resonant X-ray reflectometry (RXR) as a means to visualize charge transfer in oxide superlattices with atomic layer precision. From o…
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…
We investigated the electronic structure of the SrTiO$_3$/LaAlO$_3$ superlattice (SL) by resonant soft x-ray scattering. The (003) peak, which is forbidden for our "ideal" SL structure, was observed at all photon energies, indicating reconstruction at the interface. From the peak position analyses taking into account the effects of refraction, we obtained evidence for electronic reconstruction of Ti 3d and O $2p$ states at the interface. From reflectivity analyses, we concluded that the AlO$_2$/LaO/TiO$_2$/SrO and the TiO$_2$/SrO/AlO$_2$/LaO interfaces are quite different, leading to highly as…
Recent experiments have found new magnetic behaviors, which are different from the parent bulk materials, at the interfaces between 3$d$ and 5$d$ oxides such as SrMnO$_3$ (SMO) and SrIrO$_3$ (SIO). The system is of considerable interest due to the strong spin-orbit coupling in the 5$d$ materials on one hand and the double exchange physics in SMO on the other, which belongs to the class of the colossal magnetoresistive (CMR) manganites. In order to gain insight into the physics of the system, we have performed density-functional studies on a selected interface structure, viz., the (SMO)$_1$(SIO…
The diverse functionality emerging at oxide interfaces calls for a fundamental understanding of the mechanisms and control parameters of electronic reconstructions. Here, we explore the evolution of electronic phases in (LaAlO3)M/(SrTiO3)N(001) superlattices as a function of strain and confinement of the SrTiO3 quantum well. Density functional theory calculations including a Hubbard U term reveal a charge ordered Ti3+ and Ti4+ state for N=2 with an unanticipated orbital reconstruction, displaying alternating dxz and dyz character at the Ti3+ sites, unlike the previously reported dxy state, obt…
Dimensionality-Driven Electronic and Orbital Transitions Mediating Interfacial Magnetism in LaNiO3/CaMnO3 Observed In Situ
Temple University（天普大学）；Flatiron Institute（平顿研究所）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Cornell University（康奈尔大学）；University of California, Berkeley（加州大学伯克利分校）；Rutgers University（罗格斯大学）；Advanced Light Source, Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室先进光源中心）；Deutsches Elektronen-Synchrotron, DESY（德国电子同步辐射中心）；CNR-IOM Istituto Officina dei Materiali（意大利国家研究委员会材料研究所）；Università degli Studi di Padova（帕多瓦大学）；AREA Science Park（AREA科学园）；Columbia University（哥伦比亚大学）
In complex transition metal oxide heterostructures of physically dissimilar perovskite compounds, interface phenomena can lead to novel physical properties not observed in either of their constituents. This remarkable feature opens new prospects for technological applications in oxide electronic devices based on nm-thin oxide films. Here we report on a significant electronic charge and orbital reconstruction at interfaces between YBa2Cu3O6 and SrTiO3 studied using local spin density approximation (LSDA) with intra-atomic Coulomb repulsion (LSDA+U). We show that the interface polarity results i…
