Bilayers of the oxide 3d ferromagnet La$_{0.7}$Sr$_{0.3}$MnO$_{3}$ (LSMO) and the 5d paramagnet SrIrO$_{3}$ (SIO) with large spin-orbit coupling (SOC) have been investigated regarding the impact of interfacial SOC on magnetic order. For the growth sequence of LSMO on SIO, ferromagnetism is strongly altered and large out-of-plane-canted anisotropy associated with lacking magnetic saturation up to 4 T has been observed. Thin bilayer films have been grown coherently in both growth sequences on SrTiO$_3$ (001) by pulsed laser deposition and structurally characterized by scanning transmission electron microscopy (STEM) and x-ray diffraction (XRD). Measurements of magnetization and field-dependent Mn L$_{2,3}$ edge x-ray magnetic circular dichroism (XMCD) reveal changes of LSMO magnetic order which are strong in LSMO on SIO and weak in LSMO underneath of SIO. We attribute the impact of the growth sequence to the interfacial lattice structure/symmetry which is known to influence the interfacial magnetic coupling.
Asymmetric magnetoresistance in 3$d$-5$d$ based La$_{0.67}$Ca$_{0.33}$MnO$_3$/SrIrO$_3$ bilayer: The role of unidirectional anisotropy
Jawaharlal Nehru University（贾瓦哈拉尔·尼赫鲁大学）；Indian Institute of Technology, Hauz Khaz（印度理工学院豪兹卡兹校区）；Special Centre for Nanoscience, Jawaharlal Nehru University（贾瓦哈拉尔·尼赫鲁大学纳米科学特别中心）；UGC-DAE Consortium for Scientific Research, Indore（印度古物与考古学联合会-原子能部科学研究中心）
We study the composition dependent evolution of geometric and magnetic structures of MnO clusters within density functional theory. A systematic and extensive search through the potential energy surface is performed to identify the correct ground state, and significant isomers. We find that the magnetic structures in these MnO clusters are complex, which has been explained using the intrinsic electronic structure of the cluster, and analyzed using model Hamiltonian with parameters obtained from maximally localized Wannier functions. The calculated vertical displacement energies of off-stoichio…
Dirac semimetal strontium iridate thin films with strong spin-orbit interaction for magnetic heterostructures
Kotelnikov Institute of Radio Engineering and Electronics, Russian Academy of Sciences（俄罗斯科学院科捷利尼科夫无线电工程与电子研究所）；National Research University "Higher School of Economics", Faculty of Physics（国立研究大学高等经济大学物理系）；Moscow Institute of Physics and Technology (National Research University)（莫斯科物理技术学院（国立研究大学））
High resolution neutron diffraction shows that the mesoscopic separation into ferromagnetic (FM) and antiferromagnetic (AFM) phases and the FM transition temperature T_C in the perovskite manganite (La_{1-y}Pr_{y})_{0.7}Ca_{0.3}MnO_3 strongly depend on the quenched correlated disorder. The different disorder strengths are achieved by different procedures of the sample synthesis and quantitatively characterized by the micro-strain-type diffraction peak broadening. The system shifts to predominantly one phase state with smaller T_C as the correlated disorder strength is decreased supporting the …
Tailoring spin-orbit interactions and Coulomb repulsion are the key features to observe exotic physical phenomena such as magnetic anisotropy and topological spin texture at oxide interfaces. Our study proposes a novel platform for engineering the magnetism and spin-orbit coupling at LaMnO3/SrIrO3 (3d-5d oxide) interfaces by tuning the LaMnO3 growth conditions which controls the lattice displacement and spin-correlated interfacial coupling through charge transfer. We report on a tunable and enhanced interface-induced Rashba spin-orbit coupling and Elliot-Yafet spin relaxation mechanism in LaMn…
Electron transport coupled with magnetism has attracted attention over the years as exemplified in anomalous Hall effect due to a Berry phase in momentum space. Another type of unconventional Hall effect -- topological Hall effect, originating from the real-space Berry phase, has recently become of great importance in the context of magnetic skyrmions. We have observed topological Hall effect in bilayers consisting of ferromagnetic SrRuO$_3$ and paramagnetic SrIrO$_3$ over a wide region of both temperature and magnetic field. The topological term rapidly decreases with the thickness of SrRuO$_…
The magnetic dead layers in films a few nanometers thick are investigated for La$_{0.7}$Sr$_{0.3}$MnO$_3$ on (001)-oriented SrTiO$_3$ (STO), LaAlO$_3$ (LAO) and (LaAlO$_3$)$_{0.3}$(Sr$_2$TaAlO$_6$)$_{0.7}$ (LSAT) substrates. An anomalous moment found to persist above the Curie temperature of the La$_{0.7}$Sr$_{0.3}$MnO$_3$ films is not attributed to the films, but to oxygen vacancies at or near the surface of the substrate. The contribution to the moment from the substrate is as high as 20 $μ$B/nm$^2$ in the case of STO or LSAT. The effect is increased by adding an STO cap layer. Taking this d…
Density functional theory (DFT) calculations are used to study the magnetic and ferroelectric properties of Sr$_{1-x}$Ba$_{x}$MnO$_3$, with focus on $x=0.5$, under isotropic volume expansion/compression and biaxial strain. Our results indicate that, unexpectedly, Ba substitution alters the electronic structure in a way that, at fixed lattice parameter, notably enhances the interatomic magnetic exchange interactions. However, increasing Ba-content also causes a volume expansion which tends to weaken these interactions, leading to a net effect of weakly suppressed magnetism, as observed in exper…
We study the structural and magnetic properties of La$_{0.7}$Sr$_{0.3}$Mn$_{1-x}$Co$_x$O$_3$ ($0 \leq x \leq 1$). Rietveld refinement of X-ray Diffraction (XRD) pattern suggests phase purity of the polycrystalline samples with R$\bar{3}$c space group. Interplay of Ferromagnetic (FM) and Antiferromagnetic (AFM) interaction upon Co substitution at Mn site in La$_{0.7}$Sr$_{0.3}$MnO$_3$ is evident from magnetic measurements. There is an optimal cobalt substitution at which the coercive field is maximum.
Ca3CoMnO6 is composed of CoMnO6 chains made up of face-sharing CoO6 trigonal prisms and MnO6 octahedra. The structural, magnetic, and ferroelectric properties of this compound were investigated on the basis of density functional theory calculations. Ca3CoMnO6 is found to undergo a Jahn-Teller distortion associated with the CoO6 trigonal prisms containing high-spin Co2+ (d7) ions, which removes the C3 rotational symmetry and hence uniaxial magnetism. However, the Jahn-Teller distortion is not strong enough to fully quench the orbital moment of the high-spin Co2+ ions thereby leading to an elect…
We measured the chemical and magnetic depth profiles of a single crystalline (La$_{1-x}$Pr$_x$)$_{1-y}$Ca$_y$MnO$_{3-δ}$ (x = 0.52\pm0.05, y = 0.23\pm0.04, δ = 0.14\pm0.10) film grown on a NdGaO3 substrate using x-ray reflectometry, electron microscopy, electron energy-loss spectroscopy and polarized neutron reflectometry. Our data indicate that the film exhibits coexistence of different magnetic phases as a function of depth. The magnetic depth profile is correlated with a variation of chemical composition with depth. The thermal hysteresis of ferromagnetic order in the film suggests a first …
Manganites have been attracted considerable attention due to some intriguing magnetic properties, such as magnetoresistance, spin glass behavior and superparamagnetism. In recent years, some studies point to the effect of particle size and dimensionality of these compounds in their magnetic features. Particularly, LaCaMnO material research is well explored concerning the bulk material. To overcome the lack of the information we successfully produced advanced nanostructures of La$_{0.6}$Ca$_{0.4}$MnO$_{3}$ manganites, namely nanotubes and nanoparticles by using a sol-gel modified method, to det…
A detailed investigation of mesoscopic magnetic and crystallographic phase separation in Ca(1-x)La(x)MnO3, 0.00<=x<=0.20, is reported. Neutron powder diffraction and DC-magnetization techniques have been used to isolate the different roles played by electrons doped into the eg level as a function of their concentration x. The presence of multiple low-temperature magnetic and crystallographic phases within individual polycrystalline samples is argued to be an intrinsic feature of the system that follows from the shifting balance between competing FM and AFM interactions as a function of tempera…
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 t…
The research on multiferrocity and magnetoelectric coupling in metal-organic system is rare. Very few hybrid organic-inorganic frameworks (HOIF) exhibit direct magnetoelectric coupling (coupling between spins and dipoles) and also restricted to particular COOH-based system. We show how one can design a hybrid system to obtain such coupling based on the rational design of the organic ligands. The layered phosphonate, MnO3PC6H5.H2O, consisting of perovskite layers stacked with organic phenyl layers, is used as a starting potential candidate. To introduce dipole moment, a closely related metal-ph…
We report the study of magnetic and orbital order in Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ epitaxial thin films grown on (LaAlO$_3$)$_{0.3}$-(SrAl$_{0.5}$Ta$_{0.5}$O$_3$)$_{0.7}$ (LSAT) (011)$_c$. In a new experimental approach, the polarization and energy dependence of resonant soft x-ray scattering are used to reveal significant modifications of the magnetic order in the film as compared to the bulk, namely (i) a different magnetic ordering wave vector, (ii) a different magnetic easy axis and (iii) an additional magnetic reordering transition at low temperatures. These observations indicate a strong i…
In the present work, the structural, magnetic, and electronic properties of the two- and one-dimensional honeycomb structures of recently synthesized MnO [Zhang et al. Nat. Commun., 20, 1073-1078 (2021)] are investigated by using first principles calculations. Our calculations show that the single layer 2D MnO crystal has a degenerate antiferromagnetic (AFM) ground state and a relatively less favorable ferromagnetic (FM) state. In addition, magnetic anisotropy calculations unveil that the easy-axis direction for magnetism originating from unpaired electron states in manganese atoms is normal t…
Finite temperature disordered solid solutions and magnetic materials are difficult to study directly using first principles calculations, due to the large unit cells and many independent samples that are required. In this work, we develop a combined cluster expansion and atomic displacement expansion, which we fit to first principles energies, forces, and stresses. We then use the expansion to calculate thermodynamic quantities at nearly first principles levels of accuracy. We demonstrate that by treating all the relevant degrees of freedom explicitly, we can achieve improved convergence prope…
We use ab initio electronic structure calculations within the generalized gradient approximation (GGA+U) to density functional theory (DFT) to determine the microscopic exchange interactions in the series of orthorhombic rare-earth manganites, o-$R$MnO$_3$. Our motivation is to construct a model Hamiltonian (excluding effects due to spin-orbit coupling), which can provide an accurate description of the magnetism in these materials. First, we consider TbMnO$_3$, which exhibits a spiral magnetic order at low temperatures. We map the exchange couplings in this compound onto a Heisenberg Hamiltoni…
Multiferroics, where two or more ferroic order parameters coexist, is one of the hottest fields in condensed matter physics and materials science[1-9]. However, the coexistence of magnetism and conventional ferroelectricity is physically unfavoured[10]. Recently several remedies have been proposed, e.g., improper ferroelectricity induced by specific magnetic[6] or charge orders[2]. Guiding by these theories, currently most research is focused on frustrated magnets, which usually have complicated magnetic structure and low magnetic ordering temperature, consequently far from the practical appli…
The structural and magnetic properties of the face-centered cubic double perovskite Ba2MnWO6 were investigated using neutron powder diffraction, DC-magnetometry, muon spin relaxation and inelastic neutron scattering. Ba2MnWO6 undergoes Type II long-range antiferromagnetic ordering at a Neel temperature of 8(1) K with a frustration index, f = 8. Inelastic neutron scattering was used to identify the magnetic coupling constants J1 and J2, which were found to equal -0.080 meV and -0.076 meV respectively. This indicated that both of the magnetic coupling constants were antiferromagnetic with simila…
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…
To understand the near-interface magnetism in manganites, uniform, ultra-thin films of La_{0.67}Sr_{0.33}MnO_3 were grown epitaxially on single crystal (001) LaAlO_3 and (110) NdGaO_3 substrates. The temperature and magnetic field dependent film resistance is used to probe the film's structural and magnetic properties. A surface and/or interface related dead-layer is inferred from the thickness dependent resistance and magnetoresistance. The total thickness of the dead layer is estimated to be $\sim 30 Å$ for films on NdGaO_3 and $\sim 50 Å$ for films on LaAlO_3.
We investigate the possibility of controlling the magnetic phase transition of the heterointerface between a half-doped manganite La$_{0.5}$Ca$_{0.5}$MnO$_{3}$ and a multiferroic BiFeO$_{3}$ through magnetoelectric coupling. Using macroscopic magnetometry and element-selective x-ray magnetic circular dichroism at the Mn and Fe \emph{L}-edges, we discover that the ferroelectric polarization of BFO controls simultaneously the magnetization of BFO and LCMO. X-ray absorption spectra at oxygen \emph{K}-edge and linear dichroism at Mn \emph{L}-edge suggest that the interfacial coupling is mainly der…
