Oxide heterointerfaces constitute a rich platform for realizing novel functionalities in condensed matter. A key aspect is the strong link between structural and electronic properties, which can be modified by interfacing materials with distinct lattice symmetries. Here we determine the effect of the cubic-tetragonal distortion of $\text{SrTiO}_3$ on the electronic properties of thin films of $\text{SrIrO}_3$, a topological crystalline metal hosting a delicate interplay between spin-orbit coupling and electronic correlations. We demonstrate that below the transition temperature at 105 K, $\text{SrIrO}_3$ orthorhombic domains couple directly to tetragonal domains in $\text{SrTiO}_3$. This forces the in-phase rotational axis to lie in-plane and creates a binary domain structure in the $\text{SrIrO}_3$ film. The close proximity to the metal-insulator transition in ultrathin $\text{SrIrO}_3$ causes the individual domains to have strongly anisotropic transport properties, driven by a reduction of bandwidth along the in-phase axis. The strong structure-property relationships in perovskites make these compounds particularly suitable for static and dynamic coupling at interfaces, providing a promising route towards realizing novel functionalities in oxide heterostructures.
By means of ab initio calculations, we study the effect of charge transfer and symmetry mismatch on the magnetic and electronic properties of CaMnO$_3$ ultrathin films, epitaxially grown on SrTiO$_3$ (001). We find that the interplay of these degrees of freedom, together with the low dimensionality and the strain imposed by the substrate, changes the bulk occupancy of the Mn e_$g$ orbitals, which determines the magnetic configuration of the ultrathin CMO films. A transition from an insulating G-type to a metallic A-type antiferromagnetic configuration is stabilized.
The ferroelectric (FE) control of electronic transport is one of the emerging technologies in oxide heterostructures. Many previous studies in FE tunnel junctions (FTJs) exploited solely the differences in the electrostatic potential across the FTJs that are induced by changes in the FE polarization direction. Here, we show that in practice the junction current ratios between the two polarization states can be further enhanced by the electrostatic modification in the correlated electron oxide electrodes, and that FTJs with nanometer thin layers can effectively produce a considerably large elec…
The structures of epitaxial ultrathin Co2FeAl/MgO(001) heterostructures relating to the interface-induced perpendicular magnetic anisotropy (PMA) were investigated using scanning transmission electron microscopy, energy dispersive x-ray spectroscopy, and x-ray magnetic circular dichroism. We found that Al atoms from the Co2FeAl layer significantly interdiffuse into MgO, forming an Al-deficient Co-Fe-Al/Mg-Al-O structure near the Co2FeAl/MgO interface. This atomic replacement may play an additional role for enhancing PMA, which is consistent with the observed large perpendicular orbital magneti…
We report experimental measurements for ultrathin (< 15 nm) van der Waals heterostructures exhibiting external quantum efficiencies exceeding 50%, and show that these structures can achieve experimental absorbance > 90%. By coupling electromagnetic simulations and experimental measurements, we show that pn WSe2/MoS2 heterojunctions with vertical carrier collection can have internal photocarrier collection efficiencies exceeding 70%.
In this paper, we report the electrical and structural properties of the oxide-based metal/ferroelectric/metal (MFM) junctions. The heterostructures are composed of ultrathin layers of La0.7Ca0.3MnO3 (LCMO) as a metallic layer and, BaTiO3 (BTO) as a ferroelectric layer. Junction based devices, having the dimensions of 400 x 200 micom2, have been fabricated upon LCMO/BTO/LCMO heterostructures by photolithography and Ar-ion milling technique. The DC current-voltage (I-V) characteristics of the MFM junctions were carried out. At 300 K, the devices showed the linear (I-V) characteristics, whereas …
We fabricated ultrathin ferroelectric/correlated electron oxide heterostructures composed of the ferroelectric Pb(Zr0.2Ti0.8)O3 and the correlated electron oxide (CEO) La0.8Sr0.2MnO3 on SrTiO3 substrates by pulsed laser epitaxy. The hole accumulation in the ultrathin CEO layer was substantially modified by heterostructuring with the ferroelectric layer, resulting in an insulator-metal transition. In particular, our thickness dependent study showed that drastic changes in transport and magnetic properties were strongly coupled to the modulation of charge carriers by ferroelectric field effect, …
We have studied the chemical and electronic properties of LaAlO3/SrVO3 ultrathin films by combining hard x-ray photoemission spectroscopy and transport measurements. We compare single SrVO3 (SVO) ultrathin films and SrVO3 buried below a polar LaAlO3 (LAO) thin layer, both epitaxially grown on SrTiO3. While ultrathin films (4 unit cells) of SVO do show insulating behavior over the entire temperature range, the LAO/SVO interface has a resistivity minimum at 250 K. When increasing the SVO layer thickness, the minimum is observed to shift to higher temperatures, but the resistivity stays always sm…
Interface-Enhanced Superconductivity in Ultrathin TiN Proximitized by Topological Insulators
Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences（中国科学院宁波材料技术与工程研究所）；Eastern Institute for Advanced Study, Eastern Institute of Technology（宁波东方理工大学（暂名）先进研究院）；The Instruments Center for Physical Science, University of Science and Technology of China（中国科学技术大学物理科学仪器中心）；Key Laboratory of Functional Crystals and Laser Technology, Technical Institute of Physics and Chemistry (TIPC), Chinese Academy of Sciences（中国科学院理化技术研究所功能晶体与激光技术重点实验室）；Yongjiang Laboratory（甬江实验室）；Department of Physics & Astronomy, Rutgers, The State University of New Jersey（新泽西州立罗格斯大学物理与天文系）
Fundamental understanding of interfacial magnetic properties in ferromagnetic heterostructures is essential to utilize ferromagnetic materials for spintronic device applications. In this paper, we investigate the interfacial magnetic and electronic structures of epitaxial single-crystalline LaAlO$_3$ (LAO)/La$_{0.6}$Sr$_{0.4}$MnO$_3$ (LSMO)/Nb:SrTiO$_3$ (Nb:STO) heterostructures with varying LSMO-layer thickness, in which the magnetic anisotropy strongly changes depending on the LSMO thickness due to the delicate balance between the strains originating from both the Nb:STO and LAO layers, usin…
Structural, electronic and dielectric properties of high-quality ultrathin BaTiO3 films are investigated. The films, which are grown by ozone-assisted molecular beam epitaxy on Nb-doped SrTiO3 (001) substrates and having thicknesses as thin 8 unit cells (3.2 nm), are unreconstructed and atomically smooth with large crystalline terraces. A strain-driven transition to 3D island formation is observed for films of of 13 unit cells thickness (5.2 nm). The high structural quality of the surfaces, together with the dielectric properties similar to bulk BaTiO3 and dominantly TiO2 surface termination, …
The instability of ferroelectric ordering in ultra-thin films is one of the most important fundamental issues pertaining realization of a number of electronic devices with enhanced functionality, such as ferroelectric and multiferroic tunnel junctions or ferroelectric field effect transistors. In this paper, we investigate the polarization state of archetypal ultrathin (several nanometres) ferroelectric heterostructures: epitaxial single-crystalline BaTiO$_3$ films sandwiched between the most habitual perovskite electrodes, SrRuO$_3$, on top of the most used perovskite substrate, SrTiO$_3$. We…
Through ${in~situ}$ photoemission spectroscopy, we investigated the change in the electronic and crystal structures of dimensionality-controlled VO$_2$ films coherently grown on TiO$_2$(001) substrates. In the nanostructured films, the balance between the instabilities of a bandlike Peierls transition and a Mott transition is controlled as a function of thickness. The characteristic spectral change associated with temperature-driven metal-insulator transition in VO$_2$ thick films holds down to 1.5 nm (roughly corresponding to five V atoms along the [001] direction), whereas VO$_2$ films of le…
We report on surface effects on the electronic properties of interfaces in epitaxial LaAlO$_3$/SrTiO$_3$ heterostructures. Our results are based on first-principles electronic structure calculations for well-relaxed multilayer configurations, terminated by an ultrathin LaAlO$_3$ surface layer. On varying the thickness of this layer, we find that the interface conduction states are subject to almost rigid band shifts due to a modified Fermi energy. Confirming experimental data, the electronic properties of heterointerfaces therefore can be tuned systematically by alterating the surface-interfac…
Emergence of a Helical Metal in Rippled Ultrathin Topological Insulator Sb\textsubscript{2}Te\textsubscript{3} on Graphene
Universidad de Chile（智利大学）；CEDENNA；Universidad Adolfo Ibáñez（阿道夫·伊巴涅斯大学）；Stanford University（斯坦福大学）；Universidad Técnica Federico Santa María（弗雷德里科·圣塔玛利亚技术大学）
The tetragonal phase of chromium (III) oxide, although unstable in the bulk, can be synthesized in epitaxial heterostructures. The theoretical investigation by density functional theory predicts an antiferromagnetic ground state for this compound. We demonstrate experimentally antiferromagnetism up to 40 K in ultrathin films of t-Cr2O3 by electrical measurements exploiting interface effect within a neighboring ultrathin Pt layer. We show that magnetotransport in Pt is affected by both spin-Hall magnetoresistance and magnetic proximity effect while we exclude any role of magnetism for the low-t…
The proposal that very small Néel skyrmions can form in SrRuO$_3$/SrIrO$_3$ epitaxial bilayers and that the electric field-effect can be used to manipulate these skyrmions in gated devices strongly stimulated the recent research of SrRuO$_3$ heterostructures. A strong interfacial Dzyaloshinskii-Moriya interaction, combined with the breaking of inversion symmetry, was considered as the driving force for the formation of skyrmions in SrRuO$_3$/SrIrO$_3$ bilayers. Here, we investigated nominally symmetric heterostructures in which an ultrathin ferromagnetic SrRuO$_3$ layer is sandwiched between l…
We report the experimental observation of micron-scale magnetic skyrmions at room temperature in several Pt/Co-based thin film heterostructures designed to possess a low exchange stiffness, perpendicular magnetic anisotropy, and a modest interfacial Dzyaloshinskii-Moriya interaction (iDMI). We find both experimentally and by micromagnetic and analytic modeling that the combined action of low exchange stiffness and modest iDMI eliminates the energetic penalty associated with forming domain walls in thin film heterostructures. When the domain wall energy density approaches negative values, the r…
Two-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs) are new members of the 2D materials family with wide tunability, highly dynamic structural features and excellent physical properties. Ultrathin 2D HOIPs and their heterostructures with other 2D materials have been exploited for study of new physical phenomena and novel device applications. The in-plane mechanical properties of 2D ultrathin HOIPs are critical for understanding the coupling between mechanical and other physical fields and for integrated devices applications. Here we report for the first time the in-plane mechanic…
The motion of magnetic domain walls in ultrathin magnetic heterostructures driven by current via the spin Hall torque is described. We show results from perpendicularly magnetized CoFeB|MgO heterostructures with various heavy metal underlayers. The domain wall moves along or against the current flow depending on the underlayer material. The direction to which the domain wall moves is associated with the chirality of the domain wall spiral formed in these heterostructures. The one-dimensional model is used to describe the experimental results and extract parameters such as the Dzyaloshinskii-Mo…
Tunnel-Barrier-Engineered Ultrafast Demagnetization and Spin Transport in Graphene-Based Heterostructures
S. N. Bose National Center for Basic Sciences（S.N. 玻色基础科学国家中心）；Indian Institute of Science Education and Research Kolkata（加尔各答印度科学与教育研究所）；Uppsala University（乌普萨拉大学）
Many metallic transition-metal oxides turn insulating when grown as films that are only a few unit-cells thick. The microscopic origins of these thickness induced metal-to-insulator transitions however remain under dispute. Here, we simulate the extreme case of a monolayer of an inconspicuous correlated metal -- the strontium vanadate SrVO$_3$ -- deposited on a SrTiO$_3$ substrate. Crucially, our system can have a termination to vacuum consisting of either a SrO or a VO$_2$ top layer. While we find that both lead to Mott insulating behavior at nominal stoichiometry, the phase diagram emerging …
Building on discoveries in graphene and two-dimensional (2D) transition metal dichalcogenides, van der Waals (VdW) layered heterostructures - stacks of such 2D materials - are being extensively explored with resulting new discoveries of novel electronic and magnetic properties in the ultrathin limit. Here we review a class of naturally occurring heterostructures - so called misfits - that combine disparate VdW layers with complex stacking. Exhibiting remarkable structural complexity and diversity of phenomena, misfits provide a platform on which to systematically explore the energetics and loc…
We use ultrafast x-ray diffraction to quantify the transport of energy in laser-excited nanoscale Au/Ni bilayers. Electron transport and efficient electron-phonon coupling in Ni convert the laser-deposited energy in the conduction electrons within a few picoseconds into a strong non-equilibrium between hot Ni and cold Au phonons at the bilayer interface. Modeling of the subsequent equilibration dynamics within various two-temperature models confirms that for ultrathin Au films the thermal transport is dominated by phonons instead of conduction electrons because of the weak electron-phonon coup…
Most recently, orbital-selective quantum well states of $d$ electrons have been experimentally observed in SrVO$_3$ ultrathin films [K. Yoshimatsu et. al., Science 333, 319 (2011)] and SrTiO$_3$ surfaces [A. F. Santander-Syro et. al., Nature 469, 189 (2011)]. Hitherto, one tries to explain these experiments by a nearly free electron (NFE) model, an approach widely used for delocalized electrons in semiconductor heterostructures and simple metal films. We show that a tight binding (TB) model is more suitable for describing heterostructures with more localized $d$ electrons. In this paper, we co…
Complex oxide thin films and heterostructures exhibit a profusion of exotic phenomena, often resulting from the intricate interplay between film and substrate. Recently it has become possible to isolate epitaxially grown single-crystalline layers of these materials, enabling the study of their properties in the absence of interface effects. In this work, we create ultrathin membranes of strongly correlated materials and demonstrate top-down fabrication of nanomechanical resonators made out of \ce{SrTiO3} and \ce{SrRuO3}. Using laser interferometry, we successfully actuate and measure the motio…
Interfacial thermal transport in Si/SiC and SiC/diamond heterostructures: effects of amorphous interlayers and SiC polytypes
K. N. Toosi University of Technology（K.N.托辛理工大学）；Institute for Research in Fundamental Sciences（基础科学研究所）；Imam Khomeini International University（伊玛目霍梅尼国际大学）
We have studied the magnetic layer thickness dependence of the orbital magnetic moment in magnetic heterostructures to identify contributions from interfaces. Three different heterostructures, Ta/CoFeB/MgO, Pt/Co/AlO$_x$ and Pt/Co/Pt, which possess significant interface contribution to the perpendicular magnetic anisotropy, are studied as model systems. X-ray magnetic circular dichroism spectroscopy is used to evaluate the relative orbital moment, i.e. the ratio of the orbital to spin moments, of the magnetic elements constituting the heterostructures. We find that the relative orbital moment …
Naturally occurring van der Waals crystals have brought unprecedented interest to nanomaterial researchers in recent years. So far, more than 1800 layered materials (LMs) have been identified but only a few insulating and naturally occurring LMs were deeply investigated. Phyllosilicate minerals, which are a class of natural and abundant LMs, have been recently considered as a low-cost source of insulating nanomaterials. Within this family an almost barely explored material emerges: phlogopite [KMg3(AlSi3)O10(OH)2]. Here we carry out a high throughput characterization of this LM by employing se…
Nanostructures based on buried interfaces and heterostructures are at the heart of modern semiconductor electronics as well as future devices utilizing spintronics, multiferroics, topological effects and other novel operational principles. Knowledge of electronic structure of these systems resolved in electron momentum k delivers unprecedented insights into their physics. Here, we explore 2D electron gas formed in GaN/AlGaN high-electron-mobility transistor (HEMT) heterostructures with an ultrathin barrier layer, key elements in current high-frequency and high-power electronics. Its electronic…
Prior ultralow thermal conductivity materials are not suitable for thermoelectric applications due to the limited electronic transport in the materials. Here, we present a new class of ultralow thermal conductivity materials with substantial electronic heat transport. Our samples are graphene/metal heterostructures of transferred graphene and ultrathin metal films (Pd, Au and Ni) deposited by either thermal evaporation or rf magnetron sputtering. For the evaporated samples, we achieve an ultralow thermal conductivity of 0.06 W m-1 K-1, with phonons as the dominant heat carriers. The ultralow t…
We report local probe investigations of the magnetic interaction between BiFeO3 films and a ferromagnetic Co0.9Fe0.1 layer. Within the constraints of intralayer exchange coupling in the Co0.9Fe0.1, the multiferroic imprint in the ferromagnet results in a collinear arrangement of the local magnetization and the in-plane BiFeO3 ferroelectric polarization. The magnetic anisotropy is uniaxial, and an in-plane effective coupling field of order 10 mT is derived. Measurements as a function of multiferroic layer thickness show that the influence of the multiferroic layer on the magnetic layer becomes …
Van der Waals heterostructures formed by stacking different types of 2D materials are attracting increasing attention due to new emergent physical properties such as interlayer excitons. Recently synthesized atomically thin indium selenide (InSe) and antimony (Sb) individually exhibit interesting electronic properties such as high electron mobility in the former and high hole mobility in the latter. In this work, we present a first-principles investigation on the stability and electronic properties of ultrathin bilayer heterostructures composed of InSe and Sb single layers. The calculated elec…
Insulator-to-Metal Transition via Magnetic Reconstruction at Oxide Interfaces
CAS Key Laboratory of Magnetic Materials and Devices, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences（中国科学院磁性材料与器件重点实验室，宁波材料技术与工程研究所）；Zhejiang Province Key Laboratory of Magnetic Materials and Application Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences（浙江省磁性材料与应用技术重点实验室，宁波材料技术与工程研究所）；Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；Eastern Institute of Technology（东方理工学院）；International Research Centre Magtop, Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所磁顶国际研究中心）；CNR-SPIN, UOS Salerno（意大利国家研究委员会自旋中心萨莱诺联合实验室）；Photon Science Division, Paul Scherrer Institut（保罗谢尔研究所光子科学部）；Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences（中国科学院大学材料科学与光电工程技术中心）
We investigate magnetic domain wall (MDW) dynamics induced by applied electric fields in ferromagnetic-ferroelectric thin-film heterostructures. In contrast to conventional driving mechanisms where MDW motion is induced directly by magnetic fields or electric currents, MDW motion arises here as a result of strong pinning of MDWs onto ferroelectric domain walls (FDWs) via local strain coupling. By performing extensive micromagnetic simulations, we find several dynamical regimes, including instabilities such as spin wave emission and complex transformations of the MDW structure. In all cases, th…
Recent advances in the understanding of spin orbital effects in ultrathin magnetic heterostructures have opened new paradigms to control magnetic moments electrically. The Dzyaloshinskii-Moriya interaction (DMI) is said to play a key role in forming a Neel-type domain wall that can be driven by the spin Hall torque, a torque resulting from the spin current generated in a neighboring non-magnetic layer via the spin Hall effect. Here we show that the strength and sign of the DMI can be changed by modifying the adjacent heavy metal underlayer (X) in perpendicularly magnetized X|CoFeB|MgO heterstr…
We apply both analytical and ab-initio methods to explore heterostructures composed of a threedimensional topological insulator (3D TI) and an ultrathin normal insulator (NI) overlayer as a proof ground for the principles of the topological phase engineering. Using the continual model of a semi-infinite 3D TI we study the surface potential (SP) effect caused by an attached ultrathin layer of 3D NI on the formation of topological bound states at the interface. The results reveal that spatial profile and spectrum of these near-surface states strongly depend on both the sign and strength of the S…
We report on the perpendicular magnetic anisotropy (PMA) behavior of heavy metal (HM)/ Fe alloy/MgO thin film heterostructures after an ultrathin HfO2 passivation layer is inserted between the Fe alloy and the MgO. This is accomplished by depositing one to two atomic layers of Hf onto the Fe alloy before the subsequent rf sputter deposition of the MgO layer. This Hf layer is fully oxidized during the subsequent deposition of the MgO layer, as confirmed by X-ray photoelectron spectroscopy measurements. As the result a strong interfacial perpendicular anisotropy energy density can be achieved wi…
Two-dimensional (2D) materials have recently been the focus of extensive research. By following a similar trend as graphene, other 2D materials including transition metal dichalcogenides (MX2) and metal mono-chalcogenides (MX) show great potential for ultrathin nanoelectronic and optoelectronic devices. Despite the weak nature of interlayer forces in semiconducting MX materials, their electronic properties are highly dependent on the number of layers. Using scanning tunneling microscopy and spectroscopy (STM/STS), we demonstrate the tunability of the quasiparticle energy gap of few layered gal…
Two-dimensional (2D) transition metal dichalcogenides (TMDCs) are the subject of intense investigation for applications in optics, electronics, catalysis, and energy storage. Their optical and electronic properties can be significantly enhanced when encapsulated in an environment that is free of charge disorder. Because hexagonal boron nitride (h-BN) is atomically thin, highly-crystalline, and is a strong insulator, it is one of the most commonly used 2D materials to encapsulate and passivate TMDCs. In this report, we examine how ultrathin h-BN shields an underlying MoS2 TMDC layer from the en…
We study the decay of interface induced structural and electronic relaxation effects in epitaxial LaAlO3/SrTiO3 heterostructures. The results are based on first-principles band structure calculations for a multilayer configuration with an ultrathin LaAlO3 layer sandwiched between bulk-like SrTiO3 layers. We carry out the structure optimization for the heterointerface and investigate the electronic states of the conducting interface layer, which is found to extend over two SrTiO3 unit cells. The decay of atomic displacements is analyzed as a function of the distance to the interface, and the re…
We report the structural, magnetic, and interfacial spin transport properties of epitaxial terbium iron garnet (TbIG) ultrathin films deposited by magnetron sputtering. High crystallinity was achieved by growing the films on gadolinium gallium garnet (GGG) substrates either at high temperature, or at room temperature followed by thermal annealing, above 750 °C in both cases. The films display large perpendicular magnetic anisotropy (PMA) induced by compressive strain, and tunable structural and magnetic properties through growth conditions or the substrate lattice parameter choice. The ferrima…
Talc is an insulating layered material that is stable at ambient conditions and has high-quality basal cleavage, which is a major advantage for its use in van der Waals heterostructures. Here, we use near-field synchrotron infrared nanospectroscopy, Raman spectroscopy, and first-principles calculations to investigate the structural and vibrational properties of talc crystals, ranging from monolayer to bulk, in the 300-750 cm-1 and <60 cm-1 spectral windows. We observe a symmetry crossover from mono to bilayer talc samples, attributed to the stacking of adjacent layers. The in-plane lattice par…
MXene and its derivatives have attracted considerable attention for potential application in energy storage like batteries and supercapacitors owing to its ultrathin metallic structures. However, the complexity of the ionic and electronic dynamics in MXene based hybrids, which are normally needed for device integration, triggers both challenges and opportunities for its application. In this paper, as a prototype of metallic hybrids of MXene, heterostructures consisting of Ti3C2T2 (T= None, O and F atoms) and metallic MoS2 (1T phase) are investigated. Through density functional theory, we inves…
