Alessandro R. Mazza, Elizabeth Skoropata, Yogesh Sharma, Jason Lapano, Thomas W. Heitmann, Brianna L. Musico, Veerle Keppens, Zheng Gai, John W. Freeland, Timot… 展开作者
Alessandro R. Mazza, Elizabeth Skoropata, Yogesh Sharma, Jason Lapano, Thomas W. Heitmann, Brianna L. Musico, Veerle Keppens, Zheng Gai, John W. Freeland, Timothy R. Charlton, Matthew J. Brahlek, Adriana Moreo, Elbio Dagotto, Thomas Z. Ward
Disorder can have a dominating influence on correlated and quantum materials leading to novel behaviors which have no clean limit counterparts. In magnetic systems, spin and exchange disorder can provide access to quantum criticality, frustration, and spin dynamics, but broad tunability of these responses and a deeper understanding of strong limit disorder is lacking. In this work, we demonstrate that high entropy oxides present an unexplored route to designing quantum materials in which the presence of strong local compositional disorder hosted on a positionally ordered lattice can be used to generate highly tunable emergent magnetic behavior--from macroscopically ordered states to frustration-driven dynamic spin interactions. Single crystal La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 films are used as a structurally uniform model system hosting a magnetic sublattice with massive microstate disorder in the form of site-to-site spin and exchange type inhomogeneity. A classical Heisenberg model is found to be sufficient to describe how compositionally disordered systems can paradoxically host long-range magnetic uniformity and demonstrates that balancing the populating elements based on their discrete quantum parameters can be used to give continuous control over ordering types and critical temperatures. Theory-guided experiments show that composite exchange values derived from the complex mix of microstate interactions can be used to design the required compositional parameters for a desired response. These predicted materials are synthesized and found to possess an incipient quantum critical point when magnetic ordering types are designed to be in direct competition; this leads to highly controllable exchange bias sensitivity in the monolithic single crystal films previously accessible only in intentionally designed bilayer heterojunctions.
Epitaxial heterostructures composed of complex oxides have fascinated researchers for over a decade as they offer multiple degrees of freedom to unveil emergent many-body phenomena often unattainable in bulk. Recently, apart from stabilizing such artificial structures along the conventional [001]-direction, tuning the growth direction along unconventional crystallographic axes has been highlighted as a promising route to realize novel quantum many-body phases. Here we illustrate this rapidly developing field of geometrical lattice engineering with the emphasis on a few prototypical examples of…
Magnetism and transport are two key functional ingredients in modern electronic devices. In oxide heterostructures, ferroelectricity can provide a new route to control these two properties via electrical operations, which is scientifically interesting and technologically important. In this Brief Review, we will introduce recent progresses on this fast developing research field. Several subtopics will be covered. First, the ferroelectric polarization tuning of interfacial magnetism will be introduced, which includes the tuning of magnetization, easy axis, magnetic phases, as well as exchange bi…
In a recent Letter [PRL, 107, 047208 (2011)], Zorko et al. report on an "unexpected inhomogeneous magnetism" related to "a peculiar fragility" of the resonating-valence-bond (RVB) electronic state in the spin-1/2 quantum magnet CuNCN. Here, we show that: i) the spin model of the anisotropic triangular lattice (ATL), as proposed by Zorko et al., does not apply to CuNCN; ii) this model does not support the proclaimed RVB ground state in the relevant parameter range; iii) the magnetic state of CuNCN is not necessarily inhomogeneous.
A variety of copper tellurium oxide minerals are known, and many of them exhibit either unusual forms of magnetism, or potentially novel spin liquid behavior. Here, I review a number of the more interesting materials with a focus on their crystalline symmetry and, if known, the nature of their magnetism. Many of these exist (so far) in mineral form only, and most have yet to have their magnetic properties studied. This means a largely unexplored space of materials awaits our exploration.
Magnetic complex-oxide heterostructures are of keen interest because a wealth of phenomena at the interface of dissimilar materials can give rise to fundamentally new physics and potentially valuable functionalities. Altered magnetization, novel magnetic coupling and emergent interfacial magnetism at the epitaxial layered-oxide interfaces are under intensive investigation, which shapes our understanding on how to utilize those materials, particularly for spintronics. Neutron and x-ray based techniques have played a decisive role in characterizing interfacial magnetic structures and clarifying …
Taking into account Goodenough's superexchange rules, including both full structural relaxation and spin-orbit coupling, and checking strong correlation effects, we look for compensated half metals within the class of oxide double perovskites materials. Identifying likely half metallic (or half semimetallic) antiferromagnets, the full complications including orbital magnetism are included in order to arrive at realistic predictions of designed magnetic compounds with (near) vanishing net moment. After sorting through several candidates that have not been considered previously, two materials, K…
We investigate the magnetism in graphite by controlled oxidation. Our approach renders graphite an insulator while maintaining its structure. Fourier transform infrared spectroscopy and X-ray absorption near edge structure spectra reveal that graphite oxide has epoxy groups on its surface and it is not thermally stable. Magnetic susceptibility data exhibit negative Curie temperature, field irreversibility, and slow relaxation. The magnetic properties diminish after the epoxy groups are destroyed. The overall results indicate the unexpected magnetism is associated with the presence of epoxy gro…
We have investigated the magnetic properties of CuNCN, the first nitrogen-based analogue of cupric oxide, CuO. Our muon spin relaxation, nuclear magnetic resonance and electron spin resonance studies reveal that classical magnetic ordering is absent down to lowest temperatures. However, large enhancement of spin correlations and unexpected inhomogeneous magnetism have been observed below 80 K. We attribute this to a peculiar fragility of the electronic state against weak perturbations due to geometrical frustration, which selects between competing spin-liquid and more conventional frozen state…
We investigated the electronic and magnetic properties of the pyrochlore oxide Cd$_2$Os$_2$O$_7$ using the density-functional theory plus on-site repulsion ($U$) method, and depict the ground-state phase diagram with respect to $U$. We conclude that the all-in/all-out non-collinear magnetic order is stable in a wide range of $U$. We also show that the easy-axis anisotropy arising from the spin-orbit (SO) coupling plays a significant role in stabilizing the all-in/all-out magnetic order. A \textit{pseudo gap} was observed near the transition between the antiferromagnetic metallic and insulating…
We studied the nano-scale structure of the short-range incommensurate magnetic order in La1.5Sr0.5CoO4 by elastic neutron scattering. We find that magnetic diffuse scattering is isotropic in the a-b plane, in contrast with the naive expectation based on the popular stripe model. Indeed, charge segregation into lines favoring certain lattice direction(s) would facilitate linear stacking faults in an otherwise robust antiferromagnetism of un-doped material, leading to anisotropic disorder, with a characteristic symmetry pattern present in the neutron scattering data.
Understanding the controlling principles of band gaps trends in d electron perovskites is needed both for gauging metal-insulator transitions, as well as their application in catalysis and doping. The magnitude of this band gap is rather different for different magnetic spin configurations. We find via electronic structure theory that the factors that connect gapping magnitudes to magnetism depend on the nature of the band edge orbital character (BEOC) and surprisingly scale with the number of antiferromagnetic contacts z$_i$ between neighboring transition metal ions. The dependence is weak wh…
We have developed the crystal-field approach with strong electron correlations, extended to the Quantum Atomistic Solid-State theory (QUASST), as a physically relevant theoretical model for the description of electronic and magnetic properties of 3d-atom compounds. Its applicability has been illustrated for LaCoO3, FeBr2 and Na2V3O7. According to the QUASST theory in compounds containing open 3d-/4f-/5f-shell atoms the discrete atomic-like low-energy electronic structure survives also when the 3d atom becomes the full part of a solid matter. This low-energy atomic-like electronic structure, be…
The title quasi-1D copper oxides (0=< x =<0.4) were investigated by neutron diffraction and magnetic susceptibility studies. Polyhedral CuO4 units in the compounds were found to comprise linear-chains at inter-chain distance of approximately 10 A. The parent chain compound (x = 0), however, shows less anisotropic magnetic behavior above 2 K, although it is of substantially antiferromagnetic (mu_{eff}= 1.85 mu_{B} and Theta_{W} = -46.4 K) spin-chain system. A magnetic cusp gradually appears at about 100 K in T vs chi with the Bi substitution. The cusp (x = 0.4) is fairly characterized by and th…
Possible ferromagnetism induced in otherwise non-magnetic materials has been motivating intense research in complex oxide heterostructures. Here we show that a confined magnetism is realized at the interface between SrTiO3 and two insulating polar oxides, BiMnO3 and LaAlO3. By using polarization dependent x-ray absorption spectroscopy, we find that in both cases the magnetic order is stabilized by a negative exchange interaction between the electrons transferred to the interface and local magnetic moments. These local magnetic moments are associated to Ti3+ ions at the interface itself for LaA…
We construct the general free energy governing long-wavelength magnetism in two-dimensional oxide heterostructures, which applies irrespective of the microscopic mechanism for magnetism. This leads, in the relevant regime of weak but non-negligible spin-orbit coupling, to a rich phase diagram containing in-plane ferromagnetic, spiral, cone, and skyrmion lattice phases, as well as a nematic state stabilized by thermal fluctuations. The general conclusions are vetted by a microscopic derivation for a simple model with Rashba spin-orbit coupling.
Several puzzling aspects of interplay of the experimental lattice distortion and the the magnetic properties of four narrow $t_{2g}$-band perovskite oxides (YTiO$_3$, LaTiO$_3$, YVO$_3$, and LaVO$_3$) are clarified using results of first-principles electronic structure calculations. First, we derive parameters of the effective Hubbard-type Hamiltonian for the isolated $t_{2g}$ bands using newly developed downfolding method for the kinetic-energy part and a hybrid approach, based on the combination of the random-phase approximation and the constraint local-density approximation, for the screene…
The novel spin-chain cobalt oxide Sr5Pb3CoO12 [P-62m, a = 10.1093(2) A and c = 3.562 51(9) A at 295 K] is reported. Polycrystalline sample of the compound was studied by neutron diffraction (at 6 and 295 K) and magnetic susceptibility measurements (5 to 390 K). The cobalt oxide was found to be analogous to the copper oxide Sr5Pb3CoO12, which is comprised of magnetic-linear chains at inter-chain distance of 10 A. Although the cobalt oxide chains (mu_eff of 3.64 mu_B per Co) are substantially antiferromagnetic (theta_W = -38.8 K), neither low-dimensional magnetism nor long-range ordering has bee…
At interfaces between conventional materials, band bending and alignment are classically controlled by differences in electrochemical potential. Applying this concept to oxides in which interfaces can be polar and cations may adopt a mixed valence has led to the discovery of novel two-dimensional states between simple band insulators such as LaAlO3 and SrTiO3. However, many oxides have a more complex electronic structure, with charge, orbital and/or spin orders arising from correlations between transition metal and oxygen ions. Strong correlations thus offer a rich playground to engineer funct…
Magnetic order at room temperature induced by atomic lattice defects, like vacancies, interstitials or pairs of them, has been observed in a large number of different nonmagnetic hosts, such as pure graphite, oxides and silicon-based materials. High Curie temperatures and time independent magnetic response at room temperature indicate the extraordinary robustness of this new phenomenon in solid state magnetism. In this work, we review experimental and theoretical results in pure TiO$_2$ (anatase), which magnetic order can be triggered by low-energy ion irradiation. In particular, we discuss th…
We have prepared polycrystalline samples of LaSrRh$_{1-x}$Ga$_x$O$_4$ and LaSr$_{1-x}$Ca$_x$RhO$_4$,and have measured the x-ray diffraction, resistivity, Seebeck coefficient, magnetization and electron spin resonance in order to evaluate their electronic states. The energy gap evaluated from the resistivity and the Seebeck coefficient systematically changes with the Ga concentration, and suggests that the system changes from a small polaron insulator to a band insulator. We find that all the samples show Curie-Weiss-like susceptibility with a small Weiss temperature of the order of 1 K, which …
A quasi-one dimensional magnetism was discovered in the post-perovskite CaRuO3 (Ru4+: 4d4, Cmcm), which is iso-compositional with the perovskite CaRuO3 (Pbnm). An antiferromagnetic spin-chain function with -J/kB = 350 K well reproduces the experimental curve of the magnetic susceptibility vs. temperature, suggesting long-range antiferromagnetic correlations. The anisotropic magnetism is probably owing to the dyz - 2p- dzx and dzx - 2p- dyz superexchange bonds along a-axis. The Sommerfeld coefficient of the specific heat is fairly small, 0.16(2) mJ mol-1 K-2, indicating that the magnetism refle…
Complex oxide interfaces are a promising platform for studying a wide array of correlated electron phenomena in low-dimensions, including magnetism and superconductivity. The microscopic origin of these phenomena in complex oxide interfaces remains an open question. Here we investigate for the first time the magnetic properties of semi-insulating NdTiO$_3$/SrTiO$_3$ (NTO/STO) interfaces and present the first milli-Kelvin study of NTO/STO. The magnetoresistance (MR) reveals signatures of local ferromagnetic order and of spin-dependent thermally-activated transport, which are described quantitat…
A Kondo-lattice theory is applied to the crossover between local-moment magnetism for almost half fillings of electrons and itinerant-electron magnetism away from the half filling. In clean systems with no disorder, the bandwidth W^* of quasiparticles is non-zero and of the order of |J| at T=0K even in the limit of the half filling, with J the superexchange interaction constant between nearest neighbors. The so called Gutzwiller's term also contributes to W^* away from the half filling; it is approximately proportional to doping concentrations measured from the half filling. Magnetism is enhan…
We have investigated the magnetic and electrical resistance behaviour of Ca$_{3-x}$Y$_x$LiRuO$_6$. The parent compound exhibits magnetic ordering from Ru sublattice at a rather high temperature, 113 K. Though the paramagnetic Curie temperature ($θ$$_p$) is negative indicative of antiferromagnetic ordering, the large magnitude (-250 K) of $θ$$_p$ reveals complex nature of the magnetism in this compound. Ru ions appear to be in the pentavalent state. We note that the Néel temperature undergoes only a marginal reduction by Y substitution. All these compositions are found to be insulators and thus…
A theory of Kondo lattices is applied to the crossover between local-moment magnetism and itinerant-electron magnetism in the t-J model on a quasi-two dimensional lattice. The Kondo temperature T_K is defined as a characteristic temperature or energy scale of local quantum spin fluctuations. Magnetism with T_N >> T_K, where T_N is the N\eel temperature, is characterized as local-moment one, while magnetism with T_N << T_K is characterized as itinerant-electron one. The Kondo temperature, which also gives a measure of the strength of the quenching of magnetic moments, is renormalized by the Foc…
Experiments demonstrating the controlled growth of oxide heterostructures have raised the prospect of realizing topologically nontrivial states of correlated electrons in low dimensions. Here, we study heterostructures consisting of {111}-bilayers of double perovskites separated by inert band insulators. In bulk, these double perovskites have well-defined local moments interacting with itinerant electrons leading to high temperature ferromagnetism. Incorporating spin-orbit coupling in the two-dimensional honeycomb geometry of a {111}-bilayer, we find a rich phase diagram with tunable ferromagn…
Density functional theory augmented with Hubbard-$U$ corrections (DFT+$U$) is currently one of the widely used methods for first-principles electronic structure modeling of insulating transition metal oxides (TMOs). Since $U$ is relatively large compared to band widths, the magnetic excitations in TMOs are expected to be well described by a Heisenberg model. However, in practice the calculated exchange parameters $J_{ij}$ depend on the magnetic configuration from which they are extracted and on the functional used to compute them. In this work we investigate how the spin polarization dependenc…
First-principles calculations are performed to investigate f magnetism in A$_2$Ti$_2$O$_7$ (A=Eu, Gd, Tb, Dy, Ho, Er, Yb) magnetic pyrochlore oxides. The Hubbard U parameter and the relativistic spin orbit correction is applied for more accurate description of the electronic structure of the systems. It is argued that the main obstacle for first-principles study of these systems is the multi-minima solutions of their electronic configuration. Among the studied pyrochlores, Gd$_2$Ti$_2$O$_7$ shows the least multi-minima problem. The crystal electric field theory is applied for phenomenological …
This review is focused on extrinsic magnetotransport effects in ferromagnetic oxides. It consists of two parts; the second part is devoted to an overview of experimental data and theoretical models for extrinsic magnetotransport phenomena. Here a critical discussion of domain-wall scattering is given. Results on surfacial and interfacial magnetism in oxides are presented. Spin-polarized tunnelling in ferromagnetic junctions is reviewed and grain-boundary magnetoresistance is interpreted within a model of spin-polarized tunnelling through natural oxide barriers. The situation in ferromagnetic o…
The copper-oxide based high temperature superconductors have complex phase diagrams with multiple ordered phases. It even appears that the highest superconducting transition temperatures for certain cuprates are found in samples which display simultaneous onset of magnetism and superconductivity. We show here how the thermodynamics of fluid mixtures - a touchstone for chemists as well as hard and soft condensed matter physics - accounts for this startling observation, as well as many other properties of the cuprates in the vicinity of the instability towards ``striped'' magnetism.
Oxide superlattices and microstructures hold the promise for creating a new class of devices with unprecedented functionalities. Density-functional studies of the recently fabricated superlattices of lattice-matched perovskite titanates (SrTiO3)n/(LaTiO3)m reveal a classic wedge-shaped potential originating from the Coulomb potential of a charged sheet of La atoms. The potential in turn confines the electrons in the vicinity of the sheet, leading to an Airy-function localization of the electron states. Magnetism is suppressed for structures with a single LaTiO3 monolayer, while the bulk antife…
Strong Coulomb repulsion and spin-orbit coupling are known to give rise to exotic physical phenomena in transition metal oxides. Initial attempts to investigate systems where both of these fundamental interactions are comparably strong, such as 3d and 5d complex oxide superlattices, have revealed properties that only slightly differ from the bulk ones of the constituent materials. Here, we observe that the interfacial coupling between the 3d antiferromagnetic insulator SrMnO3 and the 5d paramagnetic metal SrIrO3 is enormously strong, yielding an anomalous Hall response as the result of charge …
Pyrochlore lattices, which are found in two important classes of materials -- the $A_2B_2X_7$ pyrochlore family and the $AB_2X_4$ spinel family -- are the quintessential 3-dimensional frustrated lattice architecture. While historically oxides ($X =$~O) have played the starring role in this field, the past decade has seen materials synthesis breakthroughs that have lead to the emergence of fluoride ($X =$~F) and chalcogenide ($X =$~S, Se) pyrochlore lattice materials. In this Research Update, we summarize recent progress in understanding the magnetically frustrated ground states in three famili…
The recently synthesized first 4d transition-metal oxide-hydride LaSr3NiRuO4H4 with the unusual high H:O ratio surprisingly displays no magnetic order down to 1.8 K. This is in sharp contrast to the similar unusual low-valent Ni+ - Ru2+ layered oxide LaSrNiRuO4 which has a rather high ferromagnetic (FM) ordering Curie temperature TC about 250 K. In this work, using density functional calculations with aid of crystal field level diagrams and superexchange pictures, we find that the contrasting magnetism is due to the distinct spin-orbital states of the Ru2+ ions (in addition to the common Ni+ S…
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…
The emergence of magnetism in otherwise nonmagnetic compounds and its underlying mechanisms have become the subject of intense research. Here we demonstrate that the nonmagnetic oxygen vacancies are responsible for an unconventional magnetic state common for titanate interfaces and surfaces. Using an effective multiorbital modelling, we find that the presence of localized vacancies leads to an interplay of ferromagnetic order in the itinerant t2g band and complex magnetic oscillations in the orbitally-reconstructed eg-band, which can be tuned by gate fields at oxide interfaces. The magnetic ph…
The realization of Kitaev spin liquid, where spins on a honeycomb lattice are coupled ferromagnetically by bond-dependent anisotropic interactions, has been a sought-after dream. 5d iridium oxides $α$-Li2IrO3 and $α$-Na2IrO3 with a honeycomb lattice of Jeff = 1/2 moments recently emerged as a possible materialization. Strong signature of Kitaev physics, however, was not captured. Here we report the discovery of a complex iridium oxide $β$-Li2IrO3 with Jeff = 1/2 moments on "hyper-honeycomb" lattice, a three-dimensional analogue of honeycomb lattice. A positive Curie-Weiss temperature $θ_{CW}$ …
The orbital and spin moment of the Ni2+ ion in NiO has been calculated within the quasi-atomic approach. The orbital moment of 0.46 mu_B amounts at 0 K, in the magnetically-ordered state, to about 20% of the total moment (2.45 mu_B). For this outcome, being in nice agreement with the recent experimental finding of the orbital moment, taking into account the intra-atomic spin-orbit coupling is indispensable. PACS: 75.25.+z, 75.10.Dg Keywords: Crystalline Electric Field, 3d oxides, magnetism, NiO
In the isostructural oxides Ca3CoMO6 (M = Co, Rh, Ir), the CoMO6 chains made up of face-sharing CoO6 trigonal prisms and MO6 octahedra are separated by Ca atoms. We analyzed the magnetic and electronic properties of these oxides on the basis of density functional theory calculations including on-site repulsion and spin-orbit coupling, and examined the essential one-electron pictures hidden behind results of these calculations. Our analysis reveals an intimate interplay between Jahn-Teller instability, uniaxial magnetism, spin arrangement, metal-metal interaction, and spin-orbit coupling in gov…
The electric-field control of $d$-electron magnetism in multiferroic transition metal oxides is attracting widespread interest for the underlying fundamental physics and for next generation spintronic devices. Here, we report an extensive study of the $3d$ magnetism in magnetoelectric Ga$_{0.6}$Fe$_{1.4}$O$_3$ (GFO) epitaxial films by polarization dependent x-ray absorption spectroscopy. We found a non-zero integral of the x-ray magnetic circular dichroism, with a sign depending upon the relative orientation between the external magnetic field and the crystallographic axes. %By reliably enlarg…
To efficiently manipulate magnetism is a key physical issue for modern condensed matter physics, which is also crucial for magnetic functional applications. Most previous relevant studies rely on the tuning of spin texture, while the spin orientation is often negligible. As an exception, spin-orbit coupled $J_{\rm eff}$ states of $4d$/$5d$ electrons provide an ideal platform for emergent quantum effects. However, many expectations have not been realized due to the complexities of real materials. Thus the pursuit for more ideal $J_{\rm eff}$ states remains ongoing. Here a near-ideal $J_{\rm eff…
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…
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)
Spinel oxides are an ideal setting to explore the interplay between configurational entropy, site selectivity, and magnetism in high entropy oxides. In this work we characterize the magnetic properties of the spinel (Cr,Mn,Fe,Co,Ni)$_3$O$_4$ and study the evolution of its magnetism as a function of non-magnetic gallium substitution. Across the range of compositions studied here, from 0% to 40% Ga, magnetic susceptibility and powder neutron diffraction measurements show that ferrimagnetic order is robust in the spinel HEO. However, we also find that the ferrimagnetic order is highly tunable, wi…
Complex oxide interfaces have been one of the central focuses in condensed matter physics and material science. Over the past decade, aberration corrected scanning transmission electron microscopy and spectroscopy has proven to be invaluable to visualize and understand the emerging quantum phenomena at an interface. In this paper, we briefly review some recent progress in the utilization of electron microscopy to probe interfaces. Specifically, we discuss several important challenges for electron microscopy to advance our understanding on interface phenomena, from the perspective of variable t…
Intensive studies of the interplay between spin-orbit coupling (SOC) and electronic correlations in transition metal compounds have recently been undertaken. In particular, $j_{\rm eff}$ = 1/2 bands on a honeycomb lattice provide a pathway to realize Kitaev's exactly solvable spin model. However, since current wisdom requires strong atomic SOC to make $j_{\rm eff}=1/2$ bands, studies have been limited to iridium oxides. Contrary to this expectation, we demonstrate how Kitaev interactions arise in 4$d$-orbital honeycomb $α$-RuCl$_3$, despite having significantly weaker SOC than the iridium oxid…
Finding new collective electronic states in materials is one of the fundamental goals of condensed matter physics. Atomic-scale superlattices formed from transition metal oxides are a particularly appealing hunting ground for new physics. In bulk form, transition metal oxides exhibit a remarkable range of magnetic, superconducting, and multiferroic phases that are of great scientific interest and are potentially capable of providing innovative energy, security, electronics and medical technology platforms. In superlattices new states may emerge at the interfaces where dissimilar materials meet…
Recent advances in creating complex oxide heterostructures, interfaces formed between two different transition metal oxides, have heralded a new era of materials and physics research, enabling a uniquely diverse set of coexisting physical properties to be combined with an ever- increasing degree of experimental control. Already, these systems have exhibited such varied phenomena as superconductivity, magnetism, and ferroelasticity, all of which are gate-tunable, demonstrating their promise for fundamental discovery and technological innovation alike. To fully exploit this richness, it is neces…
Incorporation of magnetism in graphene based compounds holds great promise for potential spintronic applications. By optimizing point defects and high edge density of defects, we report many-fold increase in the ferromagnetic saturation moment in lacey reduced graphene oxide nanoribbons (LRGONR) as compared to other graphene derivatives. The samples were synthesized using chemical unzipping methodology. Detailed structural and morphological characterizations are discussed that include XRD, Raman, SEM, HRTEM and XPS measurements. Brilluoin function analysis to magnetization data reflects best f…
We have calculated the discrete low-energy electronic structure in LaMnO3 originating from the atomic-like states of the strongly correlated 3d4 electronic system occurring in the Mn3+ ion. We take into account very strong intra-atomic correlations, crystal field interactions and the intra-atomic spin-orbit coupling. We calculated magnetic and paramagnetic state of LaMnO3 within the consistent description given by Quantum Atomistic Solid State Theory (QUASST). Our studies indicate that the intra-atomic spin-orbit coupling and the orbital magnetism are indispensable for the physically adequate …
Specific heat of the layered NaxCoO2 (x=0.65, 0.70 and 0.75) oxides has been measured in the temperature range of 3-360 K and magnetic field of 0 and 9 T. The analysis of data, assuming the combined effect of inter-layer superexchange and the phase separation into mesoscopic magnetic domains with localized spins embedded in a matrix with itinerant electronic character, suggests that the dominant contribution to the specific heat in the region of short-range ordering is mediated by quasi-2D antiferromagnetic clusters, perpendicular to the CoO2 layers.
Recent experiments have explored two-dimensional electron gases (2DEGs) at oxide (111) surfaces and interfaces, finding evidence for hexagonal symmetry breaking in SrTiO$_3$ at low temperature. We discuss many-body instabilities of such (111) 2DEGs, incorporating multiorbital interactions in the $t_{2g}$ manifold which can induce diverse magnetic and orbital orders. Such broken symmetries may partly account for the observed nematicity, cooperating or competing with phonon mechanisms. We present an effective field theory for the interplay of magnetism and nematic charge order, and discuss impli…