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）
Priyanka Aggarwal, Kirill B. Agapev, Sagar Sarkar, Biplab Sanyal, Igor Di Marco, Fabrizio Cossu
Increasing precision in the growth of superlattices sparks hope in applications that may arise from engineering layered structures. Heterostructuring and functionalization of magnetic oxides have been very popular due to their versatility and readiness for integration in modern electronics. In this study, we provide yet another example of this phenomenology by predicting that an insulating ferromagnetic state can be realized in superlattices of LaMnO$_3$ and SrTiO$_3$ oriented along the (111) direction. In strike contrast with respect to other orientations, these properties are not of extrinsic origin but arise from the interplay of structural order, strain and quantum confinement. The bandgap is shown to be either direct and indirect, depending on the precise composition, which can be explained in terms of the geometrical properties of (111)-oriented bilayers of LaMnO$_3$. The electronic structure shows narrow bands indicating localized $e_g$ states for all the investigated superlattices. These features and the analysis of the inter-atomic magnetic coupling suggest that the investigated superlattices behave as a Kugel-Khomskii material, at least for the explored compositions. Our results provide not only a new route to an insulating ferromagnet, but also novel insight into the intricate interplay between lattice symmetry, Hubbard physics and Hund's coupling to be exploited in next-generation spintronic applications.
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 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 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 inc…
(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.
55Mn NMR was used to study the ferromagnetic insulating state in four different manganites. In all cases the coexistence of two types of regions possessing different NMR spectra and nuclear spin dynamics was found. In the ferromagnetic insulating clusters the hopping frequency fhop of the electron holes is slower comparing to the NMR frequency fres and two lines ascribed to 3+ and 4+ valence states of Mn are observed. The relaxation rate increases rapidly with the increasing temperature, so that these spectra can no longer be observed for temperatures higher than approx 60 K. In ferromagnetic …
A spin-tunnel-junction based on manganites, with La$_{1-x}$Sr$_x$MnO$_3$ (LSMO) as ferromagnetic metallic electrodes and the undoped parent compound LaMnO$_3$ (LMO) as insulating barrier, is here theoretically discussed using double exchange model Hamiltonians and numerical techniques. For an even number of LMO layers, the ground state is shown to have anti-parallel LSMO magnetic moments. This highly resistive, but fragile, state is easily destabilized by small magnetic fields, which orient the LSMO moments in the direction of the field. The magnetoresistance associated with this transition is…
We show that an interplay of double exchange and impurity randomness can explain the competition between metal-ferromagnetic and insulating charge ordered states in doped manganites. The double exchange is simplified in the Ising type, whereas the randomness is modeled by the Falicov-Kimball binary distribution. The combined model is considered in a framework of dynamical mean-field theory. Using the Kubo-Greenwood formalism, the transport coefficients are explicitly expressed in terms of single particle spectral functions. Dividing the system into two sublattices we have pointed out a direct …
Single crystals of Nd_{1-x}Pb_{x}MnO_{3} with x=0.2 are grown by high temperature solution growth technique using PbO-PbF_{2} flux. Magnetization studies on the samples show a transition to a ferromagnetic state below T_c ~ 125 K and the resistivity measurements show it to be an insulator throughout the temperature range 50 - 300 K. Electron Paramagnetic Resonance studies have been performed for T > T_{C} with a view to comparing the results with those on metallic ferromagnetic manganites. The temperature dependence of various parameters like g-value, linewidth and intensity has been studied i…
Using inelastic neutron scattering we measured the microscopic magnetic coupling associated with the ferromagnetic (FM) clusters of the ``colossal magnetoresistance'' (CMR) compound Pr$_{0.70}$Ca$_{0.30}$MnO$_3$. When the insulating to metal (I-M) transition is induced by an external magnetic field there is a discontinuous change in the spin-wave stiffness constant. This result indicates that the probed regions undergo a first-order transition from an insulating to a metallic state, and that there are no FM metallic domains in the insulating region. We argue that the I-M transition in the CMR …
55Mn and 139La NMR measurements on a high quality single crystal of ferromagnetic (FM) La0.80Ca20MnO3 demonstrate the formation of localized Mn(3+,4+) states below 70 K, accompanied with strong anomalous increase of certain FM neutron Bragg peaks. (55,139)(1/T1) spin-lattice relaxation rates diverge on approaching this temperature from below, signalling a genuine phase transition at T(tr) approx. 70 K. The increased local magnetic anisotropy of the low temperature phase, the cooling-rate dependence of the Bragg peaks, and the observed finite size scaling of T(tr) with Ca (hole) doping, are sug…
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…
The resistivity $ρ_{dc}$ of manganites is studied using a random-resistor-network, based on phase-separation between metallic and insulating domains. When percolation occurs, both as chemical composition and temperature vary, results in good agreement with experiments are obtained. Similar conclusions are reached using quantum calculations and microscopic considerations. Above the Curie temperature, it is argued that ferromagnetic clusters should exist in Mn-oxides. Small magnetic fields induce large $ρ_{dc}$ changes and a bad-metal state with (disconnected) insulating domains.
We study theoretically the magnetic and electric properties of the interface between two antiferromagnetic and insulating manganites: La0.5Ca0.5MnO3, a strong correlated insulator, and CaMnO3, a band-insulator. We find that a ferromagnetic and metallic electron gas is formed at the interface between the two layers. We confirm the metallic character of the interface by calculating the in-plane conductance. The possibility of increasing the electron gas density by selective doping is also discussed.
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…
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…
An explanation is given for the charge order, orbital order and insulating state observed in half-doped manganese oxides, such as Nd$_{1/2}$Sr$_{1/2}$MnO$_{3}$. The competition between the kinetic energy of the electrons and the magnetic exchange energy drives the formation of effectively one-dimensional ferromagnetic zig-zag chains. Due to a topological phase factor in the hopping, the chains are intrinsically insulating and orbital-ordered. Most surprisingly, the strong Coulomb interaction between electrons on the same Mn-ion leads to the experimentally observed charge ordering. For doping l…
Colossal electroresistance (CER) has been observed in the ferromagnetic insulating (FMI) state of a manganite. Notably, the CER in the FMI state occurs in the absence of magnetoresistance (MR). Measurements of electroresistance (ER) and current induced resistivity switching have been performed in the ferromagnetic insulating state of a single crystal manganite of composition Nd$_0.7$Pb$_0.3$MnO$_3$ (NPMO30). The sample has a paramagnetic to ferromagnetic (Curie) transition temperature, Tc = 150 K and the ferromagnetic insulating state is realized for temperatures, T <~ 130 K. The colossal elec…
We investigate Luttinger Liquid superlattices, a periodic structure composed of two kinds of one-dimensional systems of interacting electrons. We calculate several properties of the low-energy sector: the effective charge and spin velocities, the compressibility, various correlation functions, the Landauer conductance and the Drude weight. The low-energy properties are subsumed into effective parameters, much like homogeneous one-dimensional systems. A generic result is the weighted average nature of these parameters, in proportion to the spatial extent of the underlying subunits, pointing to …
We show that applying strain on half-doped manganites makes it possible to tune the system to the proximity of a metal-insulator transition and thereby generate a colossal magnetoresistance (CMR) response. This phase competition not only allows control of CMR in ferromagnetic metallic manganites but can be used to generate CMR response in otherwise robust insulators at half-doping. Further, from our realistic microscopic model of strain and magnetotransport calculations within the Kubo formalism, we demonstrate a striking result of strain engineering that, under tensile strain, a ferromagnetic…
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…
By combining 5d transition-metal oxides showing pronounced spin-orbit interactions and oxide-based heterostructures, we propose rutile-based IrO2/TiO2 superlattices as promising candidates for unconventional electronic properties. By means of density-functional-theory simulations complemented with Hubbard-like corrections, we focus on the evolution of the electronic structure as a function of the IrO2 layer thickness and predict the heterostructures to exhibit a thickness-controlled metal-to-insulator transition, crucially related to the connectivity among IrO6 octahedra. The subtle interplay …
In view of recent experiments, indicating the spatial coexistence of conducting and insulating regions in the ferromagnetic metallic phase of doped manganites, we propose a refined mixed-phase description. The model is based on the competition of a double-exchange driven metallic component and a polaronic insulating component, whose volume fractions and carrier concentrations are determined self-consistently by requiring equal pressure and chemical potential. The resulting phase diagram as well as the order of the phase transition are in very good agreement with measured data. In addition, mod…
We present a study of the effect of biaxial strain on the electrical and magnetic properties of thin films of manganites. We observe that manganite films grown under biaxial compressive strain exhibit island growth morphology which leads to a non-uniform distribution of the strain. Transport and magnetic properties of these films suggest the coexistence of two different phases, a metallic ferromagnet and an insulating antiferromagnet. We suggest that the high strain regions are insulating while the low strain regions are metallic. In such non-uniformly strained samples, we observe a large magn…
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…
The fascinating phenomenon of destabilization of charge/orbital order in Nd0.5Sr0.5MnO3 with the reduction of grain size is critically investigated. Based on our magnetic and transport experiments followed by a theoretical analysis, we analyze various possible mechanisms and try to delineate a universal scenario behind this phenomenon. We, revisit this issue and discuss the overwhelming evidence from experiments on nano and bulk manganites as well as the absence of correlation between size reduction and pressure effects on manganites. We propose a phenomenological understanding on the basis of…
High resolution topographic images obtained by scanning tunneling microscope in the insulating state of Pr0.68Pb0.32MnO3 single crystals showed regular stripe-like or zigzag patterns on a width scale of 0.4 - 0.5 nm confirming a high temperature polaronic state. Spectroscopic studies revealed inhomogeneous maps of zero-bias conductance with small patches of metallic clusters on length scale of 2 - 3 nm only within a narrow temperature range close to the metal-insulator transition. The results give a direct observation of polarons in the insulating state, phase separation of nanometer-scale met…
We discuss the origin of the reentrant behaviors of insulating states above the Curie temperature of the colossal magnetoresistance manganites. We consider a system where charge ordering and ferromagnetism compete with each other. In the presence of randomness which pins charge order fluctuations, entropy-driven reentrant behaviors will appear, which explains the typical temperature dependence of the resistivity for CMR manganites.
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 detailed evolution of the magnitude of the local Jahn-Teller (JT) distortion in La_{1-x} Ca_x Mn O_3 is obtained across the phase diagram for 0 < x < 0.5 from high quality neutron diffraction data using the atomic pair distribution function (PDF) method. A local JT distortion is observed in the insulating phase for all Ca concentrations studied. However, in contrast with earlier local structure studies its magnitude is not constant, but decreases continuously with increasing Ca content. This observation is at odds with a simple small-polaron picture for the insulating state.
Femtosecond (fs)-resolved simultaneous measurements of charge and spin dynamics reveal the coexistence of two different quasi-particle excitations in colossal magneto-resistive (CMR) manganites, with {\em fs} and {\em ps} relaxation times respectively. Their populations reverse size above a {\em photoexcitation-intensity-threshold} coinciding with a "sudden" antiferro-to-ferromagnetic switching during $<$100 fs laser pulses. We present evidence that fast, metallic, mobile quasi--electrons dressed by {\em quantum spin fluctuations} coexist with slow, localized, polaronic charge carriers in non-…
Heterostructures of mixed-valence manganites are still under intense scrutiny, due to the occurrence of exotic quantum phenomena linked to electronic correlation and interfacial composition. For instance, if two anti-ferromagnetic insulators as LaMnO$_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…
We use a non-equilibrium many-body theory that engages the elements of transient coherence, correlation, and nonlinearity to describe changes in the magnetic and electronic phases of strongly correlated systems induced by femtosecond nonlinear photoexcitation. Using a generalized tight--binding mean field approach based on Hubbard operators and including the coupling of the laser field, we describe a mechanism for simultaneous insulator--to--metal and anti-- to ferro--magnetic transition to a transient state triggered by non-thermal ultrafast spin and charge coupled excitations. We demontrate,…
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…
Transport properties of manganese oxides suggest that their colossal magnetoresistance (CMR) is due to percolation between ferromagnetic metallic (FM) clusters in an antiferromagnetic insulating (AFI) matrix. We have studied small-angle neutron scattering under applied magnetic field in CMR Pr1-xCaxMnO3 crystals for x around 0.33. Quantitative analysis of the small-angle magnetic neutron scattering shows that the magnetic heterogeneities take place at different scales. At the mesoscopic scale (200nm), the inhomogeneities correspond to the percolation of the conducting ferromagnetic phase into …
We report a significant decrease in the low-temperature resistance induced by the application of an electric current on the $ab$-plane in the paramagnetic insulating (PMI) state of (La$_{0.4}$Pr$_{0.6}$)$_{1.2}$Sr$_{1.8}$Mn$_{2}$O$_{7}$. A colossal electroresistance effect attaining -95% is observed at lower temperatures. A colossal magnetoresistive step appears near 5T at low temperatures below 10K, accompanied by an ultrasharp width of the insulator-metal transition. Injection of higher currents to the crystal causes a disappearance of the steplike transition. These findings have a close rel…
The topological and thermoelectric properties of (EuO)$_{n}$/(MgO)$_{m}$(001) superlattices (SLs) are explored using density functional theory calculations including a Hubbard $U$ term together with Boltzmann transport theory. In (EuO)$_{1}$/(MgO)$_{3}$(001) SL at the lattice constant of MgO a sizable band gap of 0.51 eV is opened by spin-orbit coupling (SOC) due to a band inversion between occupied localized Eu $4f$ and $5d$ conduction electrons. This inversion between bands of opposite parity is accompanied by a spin reorientation in the spin-texture along the contour of band crossing surrou…
Measurements of the low-frequency (f<=100 kHz) permittivity and conductivity at T<= 150 K are reported for La(1-x)Ca(x)MnO(3) (0<=x<=1) and Ca(1-y)Sr(y)MnO(3) (0<=y<=0.75) having antiferromagnetic, insulating ground states covering a broad range of Mn valencies from Mn(3+) to Mn(4+). Static dielectric constants are determined from the low-T limiting behavior. With increasing T, relaxation peaks associated with charge-carrier hopping are observed in the real part of the permittivities and analyzed to determine dopant binding energies. The data are consistent with a simple model of hydrogenic im…
Understanding the coexistence of ferromagnetism and insulating behavior in manganites is an unsolved problem. We propose a localized-band model involving effective intermediate-range electron-electron (electron-hole) repulsion (attraction) generated by cooperative electron-phonon interaction. Double exchange mechanism, involving holes virtually hopping to nearest neighbors and back, produces magnetic polarons in an antiferromagnetic environment; when these magnetic polarons coalesce and percolate the system, we get a ferromagnetic insulator. Ferromagnetism gets more pronounced when the holes (…
Computational studies show the generation of large coexisting metallic and insulating clusters with equal electronic density in models for manganites. The clusters are induced by disorder on exchange and hopping amplitudes near first-order transitions of the non-disordered strongly coupled system. The random-field Ising model is used to explain the qualitative aspects of our results. Percolative characteristics are natural in this context. Our results explain the recently experimentally discovered micrometer size inhomogeneities in manganites. The conclusions are general and apply to a variety…
Doped and undoped manganites are modeled by the coupling between itinerant $e_g$ electrons and static $t_{2g}$ spins, the Jahn-Teller and breathing phonon modes, and the Coulomb interaction. We provide for a careful estimate of all parameters and solve the corresponding Hamiltonian by dynamical mean field theory. Our results for the one-electron spectrum, the optical conductivity, the dynamic and static lattice distortion, as well as the Curie temperature show the importance of all of the above ingredients for a realistic calculation as well as for describing the unusual dynamical properties o…
We investigated slow relaxations of the magnetostriction and residual magnetostriction of the phase-separated system (Eu$_{1-x}$Gd$_{x}$)$_{0.6}$Sr$_{0.4}$MnO$_3$, in which the metamagnetic transition from a paramagnetic insulating state to a ferromagnetic metallic state is accompanied by a lattice shrinkage. The relaxations are well fitted by a stretched exponential function, suggesting the strong frustraction between the double exchange interaction and Jahn-Teller effect. We have revealed that the Gd substitution suppresses the frozen phase-separated phase at low temperatures and stabilizes …
The metallic or insulating nature of the paramagnetic phase of the colossal-magnetoresistance manganites is investigated via a double exchange Hamiltonian with diagonal disorder. Mobility edge trajectory is determined with the transfer matrix method. Density of states calculations indicate that random hopping alone is not sufficient to induce Anderson localization at the Fermi level with 20-30% doping. We argue that the metal-insulator transtion is likely due to the formation of localized polarons from nonuniform extended states as the effective band width is reduced by random hoppings and ele…
The persistent proximity of insulating and metallic phases, a puzzling characterestic of manganites, is argued to arise from the self organization of the twofold degenerate e_g orbitals of Mn into localized Jahn-Teller(JT) polaronic levels and broad band states due to the large electron - JT phonon coupling present in them. We describe a new two band model with strong correlations and a dynamical mean-field theory calculation of equilibrium and transport properties. These explain the insulator metal transition and colossal magnetoresistance quantitatively, as well as other consequences of two …
In this paper we have created a strain driven single crystal like ferromagnetic insulating (FMI) state in a PLD grown thin film of low doped LCMO(X = 0.15)on NGO(100) substrate and make a thorough study of strain effects on the electric and magnetic transport of this film. We have studied and compared the FMI state, ferromagnetic transition temperature (TC), ferromagnetic insulating temperature (TFMI) and the resistivity of the film in details with bulk single crystals of X=0.18 to 0.22 doping region. We have found that TFMI and the localisation length of the carriers are increased and there i…
The gigantic decrease of resistance by an applied magnetic field, which is often referred to as colossal magnetoresistance (CMR), has been an attracting phenomenon in strongly correlated electron systems. The discovery of CMR in manganese oxide compounds has developed the science of strong coupling among charge, orbital, and spin degrees of freedom. CMR is also attracting scientists from the viewpoint of possible applications to sensors, memories, and so on. However, no application using CMR effect has been achieved so far, partly because the CMR materials which satisfy all of the required con…
The phase diagram and low temperature properties of the doped manganites A1-xBxMnO3 are discussed for the concentrations x < 0.4. The transition from insulating antiferromagnetic to metallic ferromagnetic state at x_cr = 0.16 is treated by means of percolation theory. The unifying description of insulating and metallic states is presented. The undoped manganite is a band insulator consisting of ferromagnetic layers, which are coupled antiferromagnetically along the c direction with a low Neel temperature. The metallic phase can be described by the two-band Fermi liquid picture. The behavior of…
We use resonant soft x-ray scattering (RSXS) to quantify the hole distribution in a superlattice of insulating La2CuO4 (LCO) and overdoped La_{2-x}Sr_{x}CuO4 (LSCO). Despite its non-superconducting constituents, this structure is superconducting with T_{c}=38 K. We found that the conducting holes redistribute electronically from LSCO to the LCO layers. The LCO layers were found to be optimally doped, suggesting they are the main drivers of superconductivity. Our results demonstrate the utility of RSXS for separating electronic from structural effects at oxide interfaces.
In a manganite film without quenched disorder, we show texturing in the form of insulating and metallic stripes above and below Curie temperature (Tc), respectively, by high resolution scanning tunneling microscopy/spectroscopy (STM/STS). The formation of these stripes involves competing orbital and charge orders, and are an outcome of overlapping electron wave-functions mediated by long-range lattice strain. Contrary to popular perception, electronically homogeneous stripe phase underlines the efficacy of the lattice strain in bringing about charge density modulation and in impeding the cross…
Novel ground-state spin structures in undoped and lightly-doped manganites are here investigated based on the orbital-degenerate double-exchange model, by using mean-field and numerical techniques. In undoped manganites, a new antiferromagnetic (AFM) state, called the E-type phase, is found adjacent in parameter space to the A-type AFM phase. Its structure is in agreement with recent experimental results. This insulating E-AFM state is also competing with a ferromagnetic metallic phase as well, suggesting that large magneto-resistant effects could exist even in undoped Mn oxides. For doped lay…
We have thoroughly investigated the entire magnetic states of under doped ferromagnetic insulating manganite Nd0.8Sr0.2MnO3 through temperature dependent linear and non linear complex ac magnetic susceptibility measurements. This ferromagnetic insulating manganite is found to have frequency independent ferromagnetic to paramagnetic transition temperature at around 140 K. At around 90 K (\approx T_f) the sample shows a second frequency dependent re - entrant magnetic transition as explored through complex ac susceptibility measurements. Non linear ac susceptibility measurements (higher harmonic…
The two-orbital model for manganites with both non-cooperative and cooperative Jahn-Teller phonons is studied at hole density x=0.5 using Monte Carlo techniques. The phase diagram is obtained varying the electron-phonon coupling and the $\rm t_{2g}$-spins exchange. The insulating CE-type charge- and orbital-ordered state with the $z$-axis charge $stacking$ observed in narrow-bandwidth manganites is stabilized in the simulations. Its charge gap $Δ_{\rm CO}$ is much larger than the critical temperature $\rm k_B T_{CO}$. Metallic-like A-type and ferromagnetic states are also obtained in the same …
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…
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…
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…
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 …
We report a 139La NMR investigation of low-doped insulating manganite samples (LaMnO(3+y) and La(1-x)Ca(x)MnO(3+y)) as a function of temperature. A volume fraction with fast nuclear relaxations was revealed by the inhomogeneous loss of the NMR signal over a broad temperature interval. Comparison with muSR data demonstrates that the wipe out of the 139La signal is mainly due to slowly fluctuating electric field gradients. This provides strong evidence for the slow diffusion of lattice excitations, identified with Jahn-Teller small polarons.
For the paramagnetic insulating phase in the metal-ordered manganite YBaMn2O6, the so-called CE-type of charge/orbital ordered state was observed within the monoclinic ab-plane, which is most commonly observed for the ordinary half doped manganites. However, TEM revealed a 4-fold periodicity along the c-axis, suggesting a new stacking pattern, where planes of the CE-type are built up according to the sequence [aabb...]. Interestingly, when th system enters into the antiferromagnetic state, this stacking pattern changes into [aaaa...] or [abab], suggesting close interplay between spins and orbi…
We study the transition at T=0 from a ferromagnetic insulating to a ferromagnetic metallic phase in manganites as a function of hole doping using an effective low-energy model Hamiltonian proposed by us recently. The model incorporates the quantum nature of the dynamic Jahn-Teller(JT) phonons strongly coupled to orbitally degenerate electrons as well as strong Coulomb correlation effects and leads naturally to the coexistence of localized (JT polaronic) and band-like electronic states. We study the insulator-metal transition as a function of doping as well as of the correlation strength U and …
