Understanding the air-stability of MnBi$_2$Te$_4$ thin films is crucial for the development and long-term operation of electronic devices based around magnetic topological insulators. In the present work, we study MnBi$_2$Te$_4$ thin films upon exposure to atmosphere using a combination of synchrotron-based photoelectron spectroscopy, room temperature electrical transport and atomic force microscopy to determine the oxidation process. After 2 days air exposure a 2 nm thick oxide passivates the surface, corresponding to oxidation of only the top two surface layers, with the underlying layers preserved. This protective oxide layer results in samples that still exhibit metallic conduction even after several days air exposure. Furthermore, the work function decreases from 4.4 eV for pristine MnBi$_2$Te$_4$ to 4.0 eV after the formation of the oxide, along with only a small shift in the core levels indicating minimal doping as a result of air exposure. With the oxide confined to the top surface layers, and the underlying layers preserved, it may be possible to explore new avenues in how to handle, prepare and passivate future MnBi$_2$Te$_4$ devices.
Ultrathin films of intrinsic magnetic topological insulator MnBi2Te4 exhibit fascinating quantum properties such as quantum anomalous Hall effect and axion insulator state. In this work, we systematically investigate the evolution of the electronic structure of MnBi2Te4 thin films. With increasing film thickness, the electronic structure changes from an insulator-type with a large energy gap to one with in-gap topological surface states, which is, however, still drastically different from the bulk material. By surface doping of alkali-metal atoms, a Rashba split band gradually emerges and hybr…
Using density functional theory and Monte Carlo calculations, we study the thickness dependence of the magnetic and electronic properties of a van der Waals interlayer antiferromagnet in the two-dimensional limit. Considering $\mathrm{MnBi_2Te_4}$ as a model material, we find it to demonstrate a remarkable set of thickness-dependent magnetic and topological transitions. While a single septuple layer block of $\mathrm{MnBi_2Te_4}$ is a topologically trivial ferromagnet, the thicker films made of an odd (even) number of blocks are uncompensated (compensated) interlayer antiferromagnets, which sh…
Intrinsic Even-Odd Thickness-Driven Anomalous Hall in Epitaxial MnBi2Te4 Thin Films
Oak Ridge National Laboratory（橡树岭国家实验室）；Pennsylvania State University（宾夕法尼亚州立大学）；Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室）；Argonne National Laboratory（阿贡国家实验室）；University of Pennsylvania（宾夕法尼亚大学）
Understanding the effects of interfacial modification to the functional properties of magnetic topological insulator thin films is crucial for developing novel technological applications from spintronics to quantum computing. Here, we report that a large electronic and magnetic response is induced in the intrinsic magnetic topological insulator MnBi2Te4 by controlling the propagation of surface oxidation. We show that the formation of the surface oxide layer is confined to the top 1-2 unit cells but drives large changes in the overall magnetic response. Specifically, we observe a dramatic reve…
A central theme in condensed matter physics is to create and understand the exotic states of matter by incorporating magnetism into topological materials. One prime example is the quantum anomalous Hall (QAH) state. Recently, MnBi2Te4 has been demonstrated to be an intrinsic magnetic topological insulator and the QAH effect was observed in exfoliated MnBi2Te4 flakes. Here, we used molecular beam epitaxy (MBE) to grow MnBi2Te4 films with thickness down to 1 septuple layer (SL) and performed thickness-dependent transport measurements. We observed a non-square hysteresis loop in the antiferromagn…
The layered antiferromagnetic MnBi2Te4 films have been proposed to be an intrinsic quantum anomalous Hall (QAH) insulator with a large gap. To realize this proposal, it is crucial to open a magnetic gap of surface states. However, recent experiments have observed gapless surface states, indicating the absence of out-of-plane surface magnetism, and thus the quantized Hall resistance can only be achieved at the magnetic field above 6 T. In this work, we propose to induce out-of-plane surface magnetism of MnBi2Te4 films via the magnetic proximity with magnetic insulator CrI3. Our calculations hav…
Through a thorough magneto-transport study of antiferromagnetic topological insulator MnBi2Te4 (MBT) thick films, a positive linear magnetoresistance (LMR) with a two-dimensional (2D) character is found in high perpendicular magnetic fields and temperatures up to at least 260 K. The nonlinear Hall effect further reveals the existence of high-mobility surface states in addition to the bulk states in MBT. We ascribe the 2D LMR to the high-mobility surface states of MBT, thus unveiling a transport signature of surface states in thick MBT films. A suppression of LMR near the Neel temperature of MB…
The intrinsic antiferromagnetic (AFM) interlayer coupling in two-dimensional magnetic topological insulator MnBi$_2$Te$_4$ places a restriction on realizing stable quantum anomalous Hall effect (QAHE) [Y. Deng et al., Science 367, 895 (2020)]. Through density functional theory calculations, we demonstrate the possibility of tuning the AFM coupling to the ferromagnetic coupling in MnBi$_2$Te$_4$ films by alloying about 50% V with Mn. As a result, QAHE can be achieved without alternation with the even or odd septuple layers. This provides a practical strategy to get robust QAHE in ultrathin MnBi…
We report direct visualization of spin-flip transition of the surface layer in antiferromagnet MnBi4Te7, a natural superlattice of alternating MnBi2Te4 and Bi2Te3 layers, using cryogenic magnetic force microscopy (MFM). The observation of magnetic contrast across domain walls and step edges confirms that the antiferromagnetic order persists to the surface layers. The magnetic field dependence of the MFM images reveals that the surface magnetic layer undergoes a first-order spin-flip transition at a magnetic field that is lower than the bulk transition, in excellent agreement with a revised Mil…
This paper discusses questions of synthesizing and pressing vanadium oxides to create film-forming materials that can be used in producing optical coatings. Based on the film-forming materials thus created, technological processes have been developed for fabricating coatings from vanadium dioxide by two methods of producing thin films: vacuum evaporation and magnetron sputtering. Questions of using films made from vanadium oxide in optical instrumentation are considered.
In this study, we report on face-centered cubic structured CoCrFeNi high-entropy alloy thin films with finely dispersed nano-oxide particles which are formed by internal oxidation. Analytical scanning transmission electron microscopy imaging found that the particles are Cr2O3. The oxide particles contribute to the hardening of the film increasing its hardness by 14% compared to that of the film without precipitates, through the Orowan-type strengthening mechanism. Our novel approach paves the way to design medium- and high-entropy alloys with high strength by making use of oxide phases.
Transition metal oxide heterostructures and interfaces host a variety of exciting quantum phases and can be grown with atomic-scale precision by utilising the intensity oscillations of $in$ $situ$ reflection high-energy electron diffraction (RHEED). However, establishing a stable oscillation pattern in the growth calibration of complex oxides films is very challenging and time consuming. Here, we develop a substantially more efficient and reliable growth calibration method for complex oxide films using molecular beam epitaxy.
The structure of thin terminated Bi(1 1 1) films of approximately 1 nm thickness is investigated from first principles. Our density functional theory calculations show that covalent bonds to the surface can change the orientation of the films completely. For thicker films, the effect is limited to the surface only. Based on these observations, we further present a simple model structure for the native oxide and chemically similar oxides, which form a protective capping layer, leaving the orientation of the films unchanged. The advantages of this energetically favorable layered termination are …
We report the epitaxial growth of Ca3SnO antiperovskite oxide films on (001)-oriented cubic yttria-stabilized zirconia (YSZ) substrates by using a conventional pulsed laser deposition (PLD) technique. In this work, a sintered Ca3SnO pellet is used as the ablation target. X-ray diffraction measurements demonstrate the (001) growth of Ca3SnO films with the antiperovskite structure and a cube-on-cube orientation relationship to the YSZ substrate. The successful synthesis of the antiperovskite phase is further confirmed by x-ray photoemission spectroscopy. These results strongly suggest that antip…
Ordering of mobile defects in functional materials can give rise to fundamentally new phases possessing ferroic and multiferroic functionalities. Here we develop the Landau theory for strain induced ordering of defects (e.g. oxygen vacancies) in thin oxide films, considering both the ordering and wavelength of possible instabilities. Using derived analytical expressions for the energies of various defect-ordered states, we calculated and analyzed phase diagrams dependence on the film-substrate mismatch strain, concentration of defects, and Vegard coefficients. Obtained results open possibiliti…
Order-disorder processes fundamentally determine the structure and properties of many important oxide systems for energy and computing applications. While these processes have been intensively studied in bulk materials, they are less investigated and understood for nanostructured oxides in highly non-equilibrium conditions. These systems can now be realized through a range of deposition techniques and probed at exceptional spatial and chemical resolution, leading to a greater focus on interface dynamics. Here we survey a selection of recent studies of order-disorder behavior at thin film oxide…
The effects of wet chemical processing conventionally employed in device fabrication standards are systematically studied on molybdenum oxide (MoOx) ultra-thin films. We have combined x-ray photoelectron spectroscopy (XPS), angle resolved XPS and x-ray reflectivity techniques to provide deep insights into the changes in composition, structure and electronic states upon treatment of films with different initial stoichiometry prepared by reactive sputtering. Our results show significant reduction effects associated with the development of gap states in MoOx, as well as changes in the composition…
The observation of ferroelectric, ferromagnetic and ferroelastic phases in thin films of binary oxides attract the broad interest of scientists and engineers. However, the theoretical consideration of observed behaviour physical nature was performed mainly for HfO2 thin films from the first principles, and in the framework of Landau-Ginzburg-Devonshire (LGD) phenomenological approach with a special attention to the role of oxygen vacancies in both cases. Allowing for generality of the LGD theory we applied it to the group of binary oxides in this work. The calculations have been performed in t…
Recently high density (HD) nonmagnetic (NM) cobalt has been discovered in a cobalt thin film, grown on Si(111). This cobalt film had a natural cobalt oxide at the top. The oxide layer forms when the film is taken out of the electron-beam deposition chamber and exposed to air. Thin HD NM cobalt layers were found near the cobalt/silicon and the cobalt-oxide/cobalt interfaces, while the thicker mid-depth region of the film was hcp cobalt with normal density and normal magnetic moment. If an ultrathin film of gold is grown on the cobalt layer, before exposing it to air, the oxidation of the cobalt…
Oxide passive films are a key for the durability of metals and alloys components as well as a central issue in corrosion science and engineering. Herein, we discuss current developments of the nanometer and sub-nanometer scale knowledge of the barrier properties and adsorption properties of passive oxide films brought by recent model experimental and theoretical investigations. The discussed aspects include (i) the chromium enrichment and its homogeneity at the nanoscale in passive films formed on Cr-bearing alloys such as stainless steel, (ii) the corrosion properties of grain boundaries in e…
