The van der Waals material CeOI is predicted to be a layered antiferromagnetic Mott insulator by DFT+U calculation. We successfully grow the CeOI films down to monolayer on graphene/6H-SiC(0001) substrate by using molecular beam epitaxy. Films are studied by {\it in-situ} scanning tunneling microscopy and spectroscopy, which shows a band gap of 4.4 eV. A metallic phase with composition unidentified also exists. This rare earth oxyhalide adds a new member to the two-dimensional magnetic materials.
Epitaxial strain has been shown to drive structural phase transitions along with novel functionalities in perovskite-based thin-films. Aliovalent doping at the A-site can drive an insulator-to-metal and magnetic transitions in perovskites along with a variety of interesting structural and electronic phenomena. Using first-principles calculations, we demonstrate here, how coupling epitaxial strain with A-site hole doping in a multiferroic double perovskite, Bi2FeCrO6, could lead to mitigation of issues related to anti-site defects and lowered magnetisation in thin-films of the material. We also…
The metal insulator transition (MIT) in VO2 has been an important topic for recent years. It has been generally agreed that the mechanism of the MIT in bulk VO2 is considered to be a collaborative Mott-Peierls transition, however the effect of the strain on the phase transition is much more complicated. In this study the effect of the large strain on the properties of VO2 films was investigated. One remarkable result is that highly strained epitaxial VO2 thin films were rutile in the insulating state as well as in the metallic state. These highly strained VO2 films underwent an electronic phas…
High quality epitaxial Sr2IrO4 thin films with various thicknesses (9-300 nm) have been grown on SrTiO3 (001) substrates, and their electric transport properties have been investigated. All samples showed the expected insulating behavior with a strong resistivity dependence on film thickness, that can be as large as three orders of magnitude at low temperature. A close examination of the transport data revealed interesting crossover behaviors for the conduction mechanism upon variation of thickness and temperature. While Mott variable range hopping (VRH) dominated the transport for films thinn…
We present evidence of strain-induced modulation of electron correlation effects and increased orbital anisotropy in the rutile phase of epitaxial VO$_2$/TiO$_2$ films from hard x-ray photoelectron spectroscopy and soft V L-edge x-ray absorption spectroscopy, respectively. By using the U(1) slave spin formalism, we further argue that the observed anisotropic correlation effects can be understood by a model of orbital selective Mott transition at a filling that is non-integer, but close to the half-filling. Because the overlaps of wave functions between $d$ orbitals are modified by the strain, …
Using spin-assisted ab-initio random structure searches, we explore an exhaustive quantum phase diagram of archetypal interfaced Mott insulators, i.e. lanthanum-iron and lanthanum-titanium oxides. In particular, we report that the charge transfer induced by the interfacial electronic reconstruction stabilises a high spin ferrous Fe2+ state. We provide a pathway to control the strength of correlation in this electronic state by tuning the epitaxial strain, yielding a manifold of quantum electronic phases, i.e. Mott-Hubbard, charge transfer and Slater insulating states. Furthermore we report tha…
High quality epitaxial thin films of Jeff=1/2 Mott insulator Sr2IrO4 with increasing in-plane tensile strain have been grown on top of SrTiO3(001) substrates. Increasing the in-plane tensile strain up to ~0.3% was observed to drop the c/a tetragonality by 1.2 %. X-ray absorption spectroscopy detected a strong reduction of the linear dichroism upon increasing in-plane tensile strain towards a reduced anisotropy in the local electronic structure. While the most relaxed thin film shows a consistent dependence with previously reported single crystal bulk measurements, electrical transport reveals …
We investigate the effect of epitaxial strain on the Mott metal-insulator transition (MIT) in perovskite systems with d^1 and d^2 electron configuration of the transition metal (TM) cation. We first discuss the general trends expected from the changes in the crystal-field splitting and in the hopping parameters that are induced by epitaxial strain. We argue that the strain-induced crystal-field splitting generally favors the Mott-insulating state, whereas the strain-induced changes in the hopping parameters favor the metallic state under compressive strain and the insulating state under tensil…
We use density functional theory plus dynamical mean-field theory (DFT+DMFT) to study multiple control parameters for tuning the metal-insulator transition (MIT) in CaVO$_3$ thin films. We focus on separating the effects resulting from substrate-induced epitaxial strain from those related to the reduced thickness of the film. We show that tensile epitaxial strain of around 3-4% is sufficient to induce a transition to a paramagnetic Mott-insulating phase. This corresponds to the level of strain that could be achieved on a SrTiO$_3$ substrate. Using free-standing slab models, we then demonstrate…
Transition metal oxides have long been an area of interest for water electrocatalysis through the oxygen evolution and oxygen reduction reactions. Iron oxides, such as LaFeO$_{3}$, are particularly promising due to the favorable energy alignment of the valence and conduction bands comprised of Fe$^{3+}$ cations and the visible light band gap of such materials. In this work, we examine the role of band alignment on the electrocatalytic oxygen evolution reaction (OER) in the intrinsic semiconductor LaFeO$_{3}$ by growing epitaxial films of varying thicknesses on Nb-doped SrTiO$_{3}$. Using cycli…
A heterojunction Mott field effect transistor (FET) is proposed that consists of an epitaxial channel material that exhibits an electron-correlation-induced Mott metal-to-insulator transition. The Mott material is remotely (modulation) doped with a degenerately doped conventional band insulator. An applied voltage modulates the electron transfer from the doped band insulator to the Mott material and produces transistor action by inducing an insulator-to-metal transition. Materials parameters from rare-earth nickelates and SrTiO3 are used to assess the potential of the "modulation-doped Mott FE…
We have synthesized thermodynamically metastable Ca2IrO4 thin-films on YAlO3 (110) substrates by pulsed laser deposition. The epitaxial Ca2IrO4 thin-films are of K2NiF4-type tetragonal structure. Transport and optical spectroscopy measurements indicate that the electronic structure of the Ca2IrO4 thin-films is similar to that of Jeff = 1/2 spin-orbit-coupled Mott insulator Sr2IrO4 and Ba2IrO4, with the exception of an increased gap energy. The gap increase is to be expected in Ca2IrO4 due to its increased octahedral rotation and tilting, which results in enhanced electron-correlation, U/W. Our…
In this paper, we have studied the effect of strain relaxation on magneto-transport properties of La_0.7Ca_0.3MnO_3 epitaxial films (200 nm thick), which were deposited by pulsed laser deposition technique under identical conditions. All the films are epitaxial and have cubic unit cell. The amount of strain relaxation has been varied by taking three different single crystal substrates of SrTiO_3, LaAlO_3 and MgO. It has been found that for thicker films the strain gets relaxed and produces variable amount of disorder depending on the strength of strain relaxation. The magnitude of lattice rela…
Perovskite LaTiO$_3$ bulk is a typical Mott-insulator with G-type antiferromagnetic order. In this work, the biaxial strain effects on the ground magnetic order of LaTiO$_3$ films grown on various substrates have been studied. For the compressive strain, LaTiO$_3$ films grown on LaAlO$_3$, LaGaO$_3$, and SrTiO$_3$ substrates undergo a phase transition from the original G-type antiferromagnet to A-type antiferromagnet. The underlying physical mechanisms are the lattice distortions tunned by strain. While for the tensile strain, the BaTiO$_3$ and LaScO$_3$ substrates have been tested, which show…
Recent progress in growth and characterization of thin-film VO$_2$ has shown its electronic properties can be significantly modulated by epitaxial matching. To throw new light on the concept of `Mott engineering', we develop a symmetry-consistent approach to treat structural distortions and electronic correlations in epitaxial VO$_2$ films under strain, and compare our design with direct experimental probes. We find strong evidence for the emergence of correlation-driven charge order deep in the metallic phase, and our results indicate that exotic phases of VO$_2$ can be controlled with epitax…
Heterointerfaces in complex oxide systems open new arenas in which to test models of strongly correlated material, explore the role of dimensionality in metal-insulator-transitions (MITs) and small polaron formation. Close to the quantum critical point Mott MITs depend on band filling controlled by random disordered substitutional doping. Delta-doped Mott insulators are potentially free of random disorder and introduce a new arena in which to explore the effect of electron correlations and dimensionality. Epitaxial films of the prototypical Mott insulator GdTiO3 are delta-doped by substituting…
We have investigated structural, transport, and optical properties of tensile strained (Sr$_{1-x}$La$_x$)$_3$Ir$_2$O$_7$ (x = 0, 0.025, 0.05) epitaxial thin-films. While High-T$_c$ superconductivity is predicted theoretically in the system, we have observed that all of the samples remain insulating with finite optical gap energies and Mott variable-range hopping characteristics in transport. Cross-sectional scanning transmission electron microscopy indicates that structural defects such as stacking faults appear in this system. The insulating behavior of the La-doped Sr$_3$Ir$_2$O$_7$ thin-fil…
High-quality epitaxial SrVO3 (SVO) thin films of various thicknesses were grown on (001)-oriented LSAT substrates by pulsed electron-beam deposition technique. Thick SVO films (~25 nm) exhibited metallic behavior with the electrical resistivity following the T2 law corresponding to a Fermi liquid system. We observed a temperature driven metal-insulator transition (MIT) in SVO ultrathin films with thicknesses below 6.5 nm, the transition temperature TMIT was found to be at 50 K for the 6.5 nm film, 120 K for the 5.7 nm film and 205 K for the 3 nm film. The emergence of the observed MIT can be a…
Resistances that exceed the Mott-Ioffe-Regel limit, known as bad metal behavior, and non-Fermi liquid behavior are ubiquitous features of the normal state of many strongly correlated materials. Here we establish the conditions that lead to bad metal and non-Fermi liquid phases in NdNiO3, which exhibits a prototype, bandwidth-controlled metal-insulator transition. We show that resistance saturation is determined by the magnitude of the Ni eg orbital splitting, which can be tuned by strain in epitaxial films, causing the appearance of bad metal behavior under certain conditions. The results shed…
Synthesis of epitaxial TaO$_2$ thin films on Al$_2$O$_3$ by suboxide molecular-beam epitaxy and thermal laser epitaxy
Cornell University（康奈尔大学）；Platform for the Accelerated Realization, Analysis, and Discovery of Interface Materials (PARADIM), Cornell University（界面材料加速实现、分析和发现平台 (PARADIM)，康奈尔大学）；Kavli Institute at Cornell for Nanoscale Science（康奈尔卡弗里纳米科学研究所）；Department of Materials Science and Engineering, Cornell University（康奈尔大学材料科学与工程系）；School of Applied and Engineering Physics, Cornell University（康奈尔大学应用工程物理学院）
We use density functional theory plus dynamical mean-field theory to demonstrate the emergence of a metallic layer at the interface between the two Mott insulators LaTiO$_3$ and LaVO$_3$. The metallic layer is due to charge transfer across the interface, which alters the valence state of the transition metal cations close to the interface. Somewhat counter-intuitively, the charge is transferred from the Ti cations with formal $d^1$ electron configuration to the the V cations with formal $d^2$ configuration, thereby increasing the occupation difference of the $t_{2g}$ states. This can be unders…
The insulator-to-metal transition in Mott insulators is the key mechanism for a novel class of electronic devices, belonging to the Mottronics family. Intense research efforts are currently devoted to the development of specific control protocols, usually based on the application of voltage, strain, pressure and light excitation. The ultimate goal is to achieve the complete control of the electronic phase transformation, with dramatic impact on the performance, for example, of resistive switching devices. Here, we investigate the simultaneous effect of external voltage and excitation by ultras…
We investigate the electronic structure of the epitaxial VO$_2$ films in the rutile phase using the density functional theory combined with the slave spin method (DFT+SS). In DFT-SS, the multiorbital Hubbard interactions are added to a DFT-fit tight-binding model, and we employ the slave-spin method to treat the electron correlation. We find that while stretching the system along the rutile $c$-axis results in a band structure favoring an anisotropic orbital fillings, the electron correlation favors an equal electron filling among $t_{2g}$ orbitals. These two distinct effects cooperatively ind…
We report a La2CuO4-like interlayer antiferromagnetic order in Sr2IrO4 films with large orthorhombic distortion (> 1.5%). The biaxial lattice strain in epitaxial heterostructures of Sr2IrO4/Ca3Ru2O7 lowers the crystal symmetry of Sr2IrO4 from tetragonal (C4) to orthorhombic (C2), guiding the Ir 5d Jeff = 1/2 pseudospin moment parallel to the elongated b-axis via magnetic anisotropy. From resonant X-ray scattering experiments, we observed an antiferromagnetic order in the orthorhombic Sr2IrO4 film whose interlayer stacking pattern is inverted from that of the tetragonal Sr2IrO4 crystal. This in…
A1-xFe2-ySe2 (A = K, Cs, Rb, Tl) are recently discovered iron-based superconductors with critical temperatures (Tc) ranging up to 32 K. Their parent phases have unique properties when compared with other iron-based superconductors; e.g., their crystal structures include ordered Fe vacancies, their normal states are antiferromagnetic (AFM) insulating phases, and they have extremely high Néel transition temperatures. However, control of carrier doping into the parent AFM insulators has been difficult due to their intrinsic phase separation. Here, we fabricated an Fe-vacancy-ordered TlFe1.6Se2 in…
Modulation of the charge carrier density in a Mott material by remote doping from a highly doped conventional band insulator is proposed to test theoretical predictions of band filling control of the Mott metal-insulator transition without introducing lattice distortions or disorder, as is the case for chemical doping. The approach is experimentally tested using ultrathin (2.5 nm) NdNiO3 films that are epitaxially grown on La-doped SrTiO3 films. We show that remote doping systematically changes the charge carrier density in the NdNiO3 film and causes a moderate shift in the metal-insulator tra…
We have investigated the electronic and optical properties of (Sr$_{1-x}$Ca$_{x}$)$_2$IrO$_4$ (x= 0 - 0.375) and (Sr$_{1-y}$Ba$_y$)$_2$IrO$_4$ (y= 0 - 0.375) epitaxial thin-films, in which the bandwidth is systematically tuned via chemical substitutions of Sr ions by Ca and Ba. Transport measurements indicate that the thin-film series exhibits insulating behavior, similar to the J$_{eff}$= 1/2 spin-orbit Mott insulator Sr$_2$IrO$_4$. As the average A-site ionic radius increases from (Sr$_{1-x}$Ca$_{x}$)$_2$IrO$_4$ to (Sr$_{1-y}$Ba$_y$)$_2$IrO$_4$, optical conductivity spectra in the near-infra…
Magnetic insulators with strong perpendicular magnetic anisotropy (PMA) play a key role in exploring pure spin current phenomena and developing ultralow-dissipation spintronic devices, thereby it is highly desirable to develop new material platforms. Here we report epitaxial growth of La2/3Sr1/3MnO3 (LSMO)-SrIrO3 (SIO) composite oxide films (LSMIO) with different crystalline orientations fabricated by sequential two-target ablation process using pulsed laser deposition. The LSMIO films exhibit high crystalline quality with homogeneous mixture of LSMO and SIO at atomic level. Ferrimagnetic and …
We present results of combined density functional theory plus dynamical mean-field theory (DFT+DMFT) calculations, which show that the Mott insulator LaTiO3 undergoes an insulator-to-metal transition under compressive epitaxial strain of about -2%. This transition is driven by strain-induced changes in the crystal-field splitting between the Ti t2g orbitals, which in turn are intimately related to the collective tilts and rotations of the oxygen octahedra in the orthorhombically distorted Pbnm perovskite structure. An accurate treatment of the underlying crystal structure is therefore crucial …
With the motive of unraveling the origin of native vacancy induced magnetization in ferroelectric perovskite oxide systems, here we explore the consequences of electronic structure modification in magnetic ordering of oxygen deficient epitaxial BaTiO$_{3-δ}$ thin films. Our adapted methodology employs state-of-the-art experimental approaches viz. photo-emission, photo-absorption spectroscopies, magnetometric measurements duly combined with first principles based theoretical methods within the frame work of density functional theory (DFT and DFT+\textit{U}) calculations. Oxygen vacancy (O$ _{V}…
We report on the epitaxial growth and surface structure of infinite-layer cuprate Sr1-xNdxCuO2 films on SrTiO3(001) substrates by combining ozone-assisted molecular beam epitaxy and in situ scanning tunneling microscopy. Careful substrate temperature and flux control has been used to achieve single-phase, stoichiometric, and c-axis oriented films. The surface of the films is usually characterized by a mixed CuO2 surface and gridlike superstructure. The superstructure exhibits a periodicity of 3.47 nm that corresponds to a coincidence lattice between the overlayer peroxide SrO2 and underlying C…
