Materials informatics exploiting machine learning techniques, e.g., Bayesian optimization (BO), has the potential to offer high-throughput optimization of thin-film growth conditions through incremental updates of machine learning models in accordance with newly measured data. Here, we demonstrated BO-based molecular beam epitaxy (MBE) of SrRuO3, one of the most-intensively studied materials in the research field of oxide electronics, mainly owing to its unique nature as a ferromagnetic metal. To simplify the intricate search space of entangled growth conditions, we ran the BO for a single condition while keeping the other conditions fixed. As a result, high-crystalline-quality SrRuO3 film exhibiting a high residual resistivity ratio (RRR) of over 50 as well as strong perpendicular magnetic anisotropy was developed in only 24 MBE growth runs in which the Ru flux rate, growth temperature, and O3-nozzle-to-substrate distance were optimized. Our BO-based search method provides an efficient experimental design that is not as dependent on the experience and skills of individual researchers, and it reduces experimental time and cost, which will accelerate materials research.
Using molecular beam epitaxy (MBE) to grow multi-elemental oxides (MEO) is generally challenging, partly due to difficulty in stoichiometry control. Occasionally, if one of the elements is volatile at the growth temperature, stoichiometry control can be greatly simplified using adsorption-controlled growth mode. Otherwise, stoichiometry control remains one of the main hurdles to achieving high quality MEO film growths. Here, we report another kind of self-limited growth mode, dubbed diffusion-assisted epitaxy, in which excess species diffuses into the substrate and leads to the desired stoichi…
Wurtzite (Ga,Mn)N films showing ferromagnetic behaviour at room temperature were successfully grown on sapphire(0001) substrates by molecular beam epitaxy using ammonia as nitrogen source. Magnetization measurements were carried out by a superconducting quantum interference device at the temperatures between 1.8K and 300K with magnetic field applied parallel to the film plane up to 7T. The magnetic-field dependence of magnetization of a (Ga,Mn)N film at 300K were ferromagnetic, while a GaN film showed Pauli paramagnetism like behaviour. The Curie temperatures of a (Ga,Mn)N film was estimated a…
Remote epitaxy on monolayer graphene is promising for synthesis of highly lattice mismatched materials, exfoliation of free-standing membranes, and re-use of expensive substrates. However, clear experimental evidence of a remote mechanism remains elusive. In many cases, due to contaminants at the transferred graphene/substrate interface, alternative mechanisms such as pinhole-seeded lateral epitaxy or van der Waals epitaxy can explain the resulting exfoliatable single-crystalline films. Here, we find that growth of the Heusler compound GdPtSb on clean graphene on sapphire substrates produces a…
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.
We demonstrate the making of BaZrS3 thin films by molecular beam epitaxy (MBE). BaZrS3 forms in the orthorhombic distorted-perovskite structure with corner-sharing ZrS6 octahedra. The single-step MBE process results in films smooth on the atomic scale, with near-perfect BaZrS3 stoichiometry and an atomically-sharp interface with the LaAlO3 substrate. The films grow epitaxially via two, competing growth modes: buffered epitaxy, with a self-assembled interface layer that relieves the epitaxial strain, and direct epitaxy, with rotated-cube-on-cube growth that accommodates the large lattice consta…
Remote epitaxy is a promising approach for synthesizing exfoliatable crystalline membranes and enabling epitaxy of materials with large lattice mismatch. However, the atomic scale mechanisms for remote epitaxy remain unclear. Here we experimentally demonstrate that GaSb films grow on graphene-terminated GaSb (001) via a seeded lateral epitaxy mechanism, in which pinhole defects in the graphene serve as selective nucleation sites, followed by lateral epitaxy and coalescence into a continuous film. Remote interactions are not necessary in order to explain the growth. Importantly, the small size …
The authors have applied positron annihilation spectroscopy to study the effect of different growth conditions on vacancy formation in In- and N-polar InN grown by plasma-assisted molecular beam epitaxy. The results suggest that the structural quality of the material and limited diffusion of surface adatoms during growth dictate the In vacancy formation in low electron-density undoped epitaxial InN, while growth conditions and thermodynamics have a less important role, contrary to what is observed in, e.g., GaN. Further, the results imply that in high quality InN, the electron mobility is like…
Epitaxial thin films of 1T-HfTe2 semimetal are grown by MBE on AlN(0001) substrates. The measured in-plane lattice parameter indicates an unstrained film which is also azimuthally aligned with the AlN substrate, albeit with an in-plane mosaic spread, as it would be expected for van der Waals epitaxy. Angle resolved photoemission spectroscopy combined with first principles electronic band structure calculations show steep linearly dispersing conduction and valence bands which cross near the Brillouin zone center, providing evidence that HfTe2 /AlN is an epitaxial topological Dirac semimetal.
N-polar GaN p-n diodes are realized on single-crystal N-polar GaN bulk wafers by plasma-assisted molecular beam epitaxy growth. The current-voltage characteristics show high-quality rectification and electroluminescence characteristics with a high on/off current ratio and interband photon emission. The measured electroluminescence spectrum is dominated by strong near-band edge emission, while deep level luminescence is greatly suppressed. A very low dislocation density leads to a high reverse breakdown electric field. The low leakage current N-polar diodes open up several potential application…
Recently, theorists have predicted many materials with a low magnetic moment and large spin-polarization for spintronic applications. These compounds are predicted to form in the inverse Heusler structure, however, many of these compounds have been found to phase segregate. In this study, ordered Cr2CoGa thin films were synthesized without phase segregation using molecular beam epitaxy. The present as-grown films exhibit a low magnetic moment from antiferromagnetically coupled Cr and Co atoms as measured with SQUID magnetometry and soft X-ray magnetic circular dichroism. Electrical measurement…
Ferromagnetic properties of In1-xMnxAs thin films were investigated. Room temperature ferromagnetic order was observed in nominally single-phase films with x = 0.01-0.10. Magnetization measurements indicated that these In1-xMnxAs samples had a Curie temperature of 333 K. The Curie temperature was independent of Mn concentration. The temperature dependent magnetization along with the magnitude of the saturation magnetization and microstructural data indicate that the source of the high-temperature ferromagnetism in single-phase films is not attributable to MnAs nanoprecipitates. The high transi…
Epitaxial thin films of the highly spin polarized Heusler compound Co2Cr0.6Fe0.4Al are deposited by dc magnetron sputtering. It is shown by XRD and TEM investigations how the use of an Fe buffer layer on MgO(100) substrates supports the growth of highly ordered Co2Cr0.6Fe0.4Al at low deposition temperatures. The as grown samples show a relatively large ordered magnetic moment of mu = 3.0mu_B/f.u. providing evidence for a low level of disorder.
Atomically thin PtSe2 films have attracted extensive research interests for potential applications in high-speed electronics, spintronics and photodetectors. Obtaining high quality, single crystalline thin films with large size is critical. Here we report the first successful layer-by-layer growth of high quality PtSe2 films by molecular beam epitaxy. Atomically thin films from 1 ML to 22 ML have been grown and characterized by low-energy electron diffraction, Raman spectroscopy and X-ray photoemission spectroscopy. Moreover, a systematic thickness dependent study of the electronic structure i…
The effect of film morphology on its surface chemistry and band structure has been analyzed for gallium nitride epitaxial films grown by molecular beam epitaxy. The film morphology has been studied using scanning electron microscopy and atomic force microscopy, and the bandstructure, defect and emission properties have been studied by X ray photoelectron spectroscopy and cathodoluminescence spectroscopy. It was found that the highly porous GaN nanowall network shows the highest relative conductivity and does not have defect related luminescence. The flatter films were more resistive and showed…
Here, we report a detailed method of growing LaAlGe, a non-magnetic Weyl semimetal, thin film on silicon(100) substrates by molecular beam epitaxy and their structural and electrical characterizations. 50 nm thick LaAlGe films were deposited and annealed for 16 hours in situ at a temperature 793 K. As-grown high-quality films showed uniform surface topography and near ideal stoichiometry with a body-centered tetragonal crystal structure. Temperature-dependent longitudinal resistivity can be understood with dominant interband s-d electron-phonon scattering in the temperature range 5-40 K. Hall …
We investigate the effect of the formation of metal droplets on the growth dynamics of InGaN by Plasma-Assisted Molecular Beam Epitaxy (PAMBE) at low temperatures (T = 450°C). We find that the presence of droplets on the growth surface strongly affects the adatom incorporation dynamics, making the growth rate a decreasing function of the overall metal flux impinging on the surface as soon as the metal dose exceeds the critical amount required for the nucleation of droplets. We explain this phenomenon via a model that takes into account droplet effects on the incorporation of metal adatoms into…
The growth of atomically-flat thin films of ferroelectric PbTiO3 on SrTiO3 substrates, using molecular beam epitaxy, is reported. The main issue in the growth of these materials is the high volatility of lead. This can be largely overcome by using PbO, instead of Pb, as a source and by using atomic oxygen during growth. The continuous decrease of the out-of-plane lattice parameter with increasing temperature in the investigated range, indicates that PbTiO3 is still ferroelectric at the growth temperature (Tg= 600oC), which agrees with the theoretical prediction of TC= 765oC (compared to TCbulk…
Hexagonal boron nitride (h-BN) is a layered two-dimensional material with properties that make it promising as a dielectric in various applications. We report the growth of h-BN films on Ni foils from elemental B and N using molecular beam epitaxy. The presence of crystalline h-BN over the entire substrate is confirmed by Raman spectroscopy. Atomic force microscopy is used to examine the morphology and continuity of the synthesized films. A scanning electron microscopy study of films obtained using shorter depositions offers insight into the nucleation and growth behavior of h-BN on the Ni sub…
MnBi2Te4 has recently been predicted and shown to be a magnetic topological insulator with intrinsic antiferromagnetic order. However, it remains a challenge to grow stoichiometric MnBi2Te4 films by molecular beam epitaxy (MBE) and to observe pure antiferromagnetic order by magnetometry. We report on a detailed study of MnBi2Te4 films grown on Si(111) by MBE with elemental sources. Films of about 100 nm thickness are analyzed in stoichiometric, structural, magnetic and magnetotransport properties with high accuracy. High-quality MnBi2Te4 films with nearly perfect septuple-layer structure are r…
We report comprehensive x-ray diffraction studies of the crystal structure and epitaxy of thin films of the topological insulator Bi2Te3 grown on Si (1 1 1). The films are single crystals of high crystalline quality, which strongly depends on that of their substrates, with in-plane epitaxial relationships of Bi2Te3 [2 1 -3 0] || Si [1 -1 0] and Bi2Te3 [0 1 -1 0] || Si [1 1 -2] along which the lattices of 1x3 Bi2Te3 and 2x2 Si supercells are well matched. As the samples age, we observe loss of crystalline Bi2Te3 film thickness accompanied with roughening of the crystalline interfaces, formation…
Bi$_2$Te$_3$ is a material with high efficiency of thermoelectric energy conversion. Recently, it was also recognized as a topological insulator, and is often used as the basis for creation of other types of topological matter. Pulsed laser deposition (PLD) is widely considered as a simple method for growing of multicomponent films, but not as a tool for van der Waals epitaxy. We demonstrate here that the van der Waals epitaxy of Bi$_2$Te$_3$ is indeed impossible in vacuum PLD, but is possible in the presence of a background gas, which is confirmed by the results of scanning tunneling microsco…
We have investigated the growth of BaTiO3 thin films deposited on pure and 1% Nb-doped SrTiO3(001) single crystals using atomic oxygen assisted molecular beam epitaxy (AO-MBE) and dedicated Ba and Ti Knudsen cells. Thicknesses up to 30 nm were investigated for various layer compositions. We demonstrate 2D growth and epitaxial single crystalline BaTiO3 layers up to 10 nm before additional 3D features appear; lattice parameter relaxation occurs during the first few nanometers and is completed at »10 nm. The presence of a Ba oxide rich top layer that probably favors 2D growth is evidenced for wel…
We studied structural, optical and magnetic properties of high-quality 5 and 15% Co-doped ZnO films grown by plasma-assisted molecular beam epitaxy (MBE) on (0001)-sapphire substrates. Magnetic force microscopy (MFM) and magnetic measurements with SQUID magnetometer show clear ferromagnetic behavior of the films up to room temperature whereas they are antiferromagnetic below 200 K approximately. Temperature dependence of the carrier mobility was determined using Raman line shape analysis of the longitudinal-optical-phonon-plasmon coupled modes. It shows that the microscopic mechanism for ferro…
Ultrathin films of Na3Bi on insulating substrates are desired for opening a bulk band gap and generating the quantum spin Hall effect from a topological Dirac semimetal, though continuous films in the few nanometer regime have been difficult to realize. Here, we utilize alternating layer molecular beam epitaxy (MBE) to achieve uniform and continuous single crystal films of Na3Bi(0001) on insulating Al2O3(0001) substrates and demonstrate electrical transport on films with 3.8 nm thickness (4 unit cells). The high material quality is confirmed through in situ reflection high-energy electron diff…
We report the influence of the In mole fraction on the material and electrical characteristics of p-i-n InxGa1-xN homojunctions (x = 0.10-0.40) synthesized by plasma-assisted molecular-beam epitaxy on GaN-on-sapphire substrates. Junctions terminated with p-InGaN present improved carrier extraction efficiency in comparison with devices capped with p-GaN, due to the deleterious effect of polarization discontinuities on the device performance. We demonstrate that the presence of Mg does not perturb the In incorporation in InGaN, and it leads to a significant reduction of the stacking fault densit…
We have carried out the growth of h-RFeO3 (001) (R=Lu, Yb) thin films on Fe3O4 (111)/Al2O3 (001) substrates, and studied the effect of the h-RFeO3 (001)/Fe3O4 (111) interfaces on the epitaxy and magnetism. The observed epitaxial relations between h-RFeO3 and Fe3O4 indicates an unusual matching of Fe sub-lattices rather than a matching of O sub-lattices. The out-of-plane direction was found to be the easy magnetic axis for h-YbFeO3 (001) but the hard axis for Fe3O4 (111) in the h-YbFeO3 (001)/Fe3O4 (111)/Al2O3 (001) films, suggesting a perpendicular magnetic alignment at the h-YbFeO3 (001)/Fe3O…
Materials with perpendicular magnetic anisotropy (PMA) effect with high Curie temperature ($T_C$) is essential in applications. In this work, $Cr_2Te_3$ thin films showing PMA with $T_C$ ranging from 165 K to 295 K were successfully grown on $Al_2O_3$ by the molecular beam epitaxy (MBE) technique. The structural analysis, magneto-transport and magnetic characterizations were conducted to study the physical origin of the improved $T_C$. In particular, ferromagnetic (FM) and antiferromagnetic (AFM) ordering competition were investigated. A phenomenological model based on the coupling degree betw…
The present study elucidates the correlation between the structural and optical properties of GaN nanowires grown on Si(111) substrate by plasma assisted molecular beam epitaxy (PA-MBE) technique under various growth conditions. GaN NWs exhibiting different shapes, sizes and distribution were grown at various substrate temperatures with same Ga-N (III-V) ratio of 0.4. We observe that sample grown at lower substrate temperature (~700 degC) results 2-dimensional island like structure with almost very little (~30%) circularity while increasing substrate temperature (>770 degC) leads to growth of …
Anti-ThCr$_2$Si$_2$ type $RE_2$O$_2$Sb ($RE$ = rare earth) with Sb square net has shown insulating conduction so far. Here we report the synthesis of La$_2$O$_2$Sb epitaxial thin films for the first time by multilayer solid-phase epitaxy. The valence state of Sb was about -2 evaluated from X-ray photoemission spectroscopy measurement, and the indirect band gap of 0.17 eV was observed. The La$_2$O$_2$Sb epitaxial thin film showed unexpectedly high electrical conduction as a narrow gap semiconductor, whose resistivity at room temperature was approximately ten-thousand-fold lower than that of La$…
Atomically thin transition metal dichalcogenide films with distorted trigonal (1T$^\prime$) phase have been predicted to be candidates for realizing quantum spin Hall effect. Growth of 1T$^\prime$ film and experimental investigation of its electronic structure are critical. Here we report the electronic structure of 1T$^\prime$-MoTe$_2$ films grown by molecular beam epitaxy (MBE). Growth of the 1T$^\prime$-MoTe$_2$ film depends critically on the substrate temperature, and successful growth of the film is indicated by streaky stripes in the reflection high energy electron diffraction and sharp …
Fe$_{3}$Si/Ge(Fe,Si)/Fe$_{3}$Si thin film stacks were grown by a combination of molecular beam epitaxy and solid phase epitaxy (Ge on Fe$_{3}$Si). The stacks were analyzed using electron microscopy, electron diffraction, and synchrotron X-ray diffraction. The Ge(Fe,Si) films crystallize in the well oriented, layered tetragonal structure FeGe$_{2}$ with space group P4mm. This kind of structure does not exist as a bulk material and is stabilized by solid phase epitaxy of Ge on Fe$_{3}$Si. We interpret this as an ordering phenomenon induced by minimization of the elastic energy of the epitaxial f…
Renewable energy sources such as solar and wind are critical to combatting global warming. Nevertheless, their intermittent energy generation requires the development of large-scale grid energy storage, in contrast to the on-demand generation of coal-based power plants. Sodium-ion batteries offer a promising potential technology, yet because sodium ions are larger than lithium ions, sodium-ion intercalation results in more drastic structural rearrangements. An improved understanding of structural dynamics and ionic diffusion pathways is crucial to developing more durable sodium-ion batteries. …
Liquid phase epitaxy of an 18 nm thick Yttrium Iron garnet (YIG) film is achieved. Its magnetic properties are investigated in the 100 -- 400 K temperature range, as well as the influence of a 3 nm thick Pt overlayer on them. The saturation magnetization and the magnetocrystalline cubic anisotropy of the bare YIG film behave similarly to bulk YIG. A damping parameter of only a few $10^{-4}$ is measured, together with a low inhomogeneous contribution to the ferromagnetic resonance linewidth. The magnetic relaxation increases upon decreasing temperature, which can be partly ascribed to impurity …
We report the interplay between In incorporation and strain relaxation kinetics in high-In-content InxGa1-xN (x = 0.3) layers grown by plasma-assisted molecular-beam epitaxy. For In mole fractions x = 0.13-0.48, best structural and morphological quality is obtained under In excess conditions, at In accumulation limit, and at a growth temperature where InGaN decomposition is active. Under such conditions, in situ and ex situ analysis of the evolution of the crystalline structure with the growth thickness points to an onset of misfit relaxation after the growth of 40 nm, and a gradual relaxation…
Hexagonal group IV materials like silicon and germanium are expected to display remarkable optoelectronic properties for future development of photonic technologies. However, the fabrication of hexagonal group IV semiconductors within the vapour-liquid-solid method has been obtained using gold as a catalyst thus far. In this letter, we show the synthesis of hexagonal Ge on self-assisted GaAs nanowires using molecular beam epitaxy. With an accurate tuning of the Ga and As molecular beam flux we selected the crystal phase, cubic or hexagonal, of the GaAs NWs during the growth. A 500 nm-long hexa…
We have synthesized Fe$_{1+y}$Te thin films by means of molecular beam epitaxy (MBE) under Te-limited growth conditions. We found that epitaxial layer-by-layer growth is possible for a wide range of excess Fe values, wider than expected from what is known on the bulk material. Using x-ray magnetic circular dichroism spectroscopy at the Fe L$_{2,3}$ and Te M$_{4,5}$ edges, we observed that films with high excess Fe contain ferromagnetic clusters while films with lower excess Fe remain nonmagnetic. Moreover, x-ray absorption spectroscopy showed that it is possible to obtain films with very simil…
In1-xMnxAs diluted magnetic semiconductor (DMS) thin films have been grown using metalorganic vapor phase epitaxy (MOVPE). Tricarbonyl(methylcyclopentadienyl)manganese was used as the Mn source. Nominally single-phase, epitaxial films were achieved with Mn content as high as x=0.14 using growth temperatures Tg>475 C. For lower growth temperatures and higher Mn concentrations, nanometer scale MnAs precipitates were detected within the In1-xMnxAs matrix. Magnetic properties of the films were investigated using a superconducting quantum interference device (SQUID) magnetometer. Room-temperature f…
We demonstrate the growth of thin films of molybdenum ditelluride and molybdenum diselenide on sapphire substrates by molecular beam epitaxy. In-situ structural and chemical analyses reveal stoichiometric layered film growth with atomically smooth surface morphologies. Film growth along the (001) direction is confirmed by X-ray diffraction, and the crystalline nature of growth in the 2H phase is evident from Raman spectroscopy. Transmission electron microscopy is used to confirm the layered film structure and hexagonal arrangement of surface atoms. Temperature dependent electrical measurements…
In many transition metal oxides (TMOs), oxygen stoichiometry is one of the most critical parameters that plays a key role in determining the structural, physical, optical, and electrochemical properties of the material. However, controlling the growth to obtain high quality single crystal films having the right oxygen stoichiometry, especially in a high vacuum environment, has been viewed as a challenge. In this work, we show that through proper control of the plume kinetic energy, stoichiometric crystalline films can be synthesized without generating oxygen defects, even in high vacuum. We us…
High-index Bi2Se3(221) film has been grown on In2Se3-buffered GaAs(001), in which a much retarded strain relaxation dynamics is recorded. The slow strain-relaxation process of in epitaxial Bi2Se3(221) can be attributed to the layered structure of Bi2Se3 crystal, where the epifilm grown along [221] is like a pile of weakly-coupled quintuple layer slabs stacked side-by-side on substrate. Finally, we have revealed the strong chemical bonding at the interface of Bi2Se3 and In2Se3 by plotting differential charge contour calculated by first-principle method. This study points to the feasibility of a…
Epitaxial growth of topological insulator Bi2Se3 thin films on nominally flat and vicinal Si(111) substrates is studied. In order to achieve planner growth front and better quality epifilms, a two-step growth method is adopted for the van der Waal epitaxy of Bi2Se3 to proceed. By employing vicinal Si(111) substrate surfaces, the in-pane growth rate anisotropy of Bi2Se3 is explored to achieve single crystalline Bi2Se3 epifilms, in which threading defects and twins are effectively suppressed. Optimization of the growth parameters has resulted in vicinal Bi2Se3 films showing a carrier mobility of…
Stoichiometric, epitaxial LaCrO3 films have been grown on TiO2-terminated SrTiO3(001) substrates by molecular beam epitaxy using O2 as the oxidant. Film growth occurred in a layer-by-layer fashion, giving rise to structurally excellent films and surfaces which preserve the step-terrace structure of the substrate. The critical thickness is in excess of 500 Å. Near-surface Cr(III) is highly susceptible to further oxidation to Cr(V), leading to the formation of a disordered phase upon exposure to atomic oxygen. Recovery of the original epitaxial LaCrO3 phase is readily achieved by vacuum annealin…
N-polar (In,Ga)N/GaN quantum wells prepared on freestanding GaN substrates by plasma-assisted molecular beam epitaxy at conventional growth temperatures of about 650 °C do not exhibit any detectable luminescence even at 10 K. In the present work, we investigate (In,Ga)N/GaN quantum wells grown on Ga- and N-polar GaN substrates at a constant temperature of 730 °C. This exceptionally high temperature results in a vanishing In incorporation for the Ga-polar sample. In contrast, quantum wells with an In content of 20% and abrupt interfaces are formed on N-polar GaN. Moreover, these quantum wells e…
Epitaxial growth of BaBiO3 thin films on SrTiO3(001) and MgO(001) substrates using molecular beam epitaxy and controlling their crystal orientations competition
Strain-engineering is a powerful means to tune the polar, structural, and electronic instabilities of incipient ferroelectrics. KTaO3 is near a polar instability and shows anisotropic superconductivity in electron-doped samples. Here, we demonstrate growth of high quality KTaO3 thin films by molecular-beam epitaxy. Tantalum was provided by both a suboxide source emanating a TaO2 flux from Ta2O5 contained in a conventional effusion cell as well as an electron-beam-heated tantalum source. Excess potassium and a combination of ozone and oxygen (10 \% O3 + 90 \% O2) were simultaneously supplied wi…
Materials with a layered Kagome lattice are expected to give rise to novel physics arising from band structures with topological properties, spin liquid behavior and the formation of skyrmions. Until now, most work on Kagome materials has been performed on bulk samples due to difficulties in thin film synthesis. Here, by using molecular beam epitaxy, layered Kagome-structured FeSn films are synthesized on (111) oriented LaAlO3 substrate. Both in-situ and ex-situ characterizations indicate these films are highly crystalline and c-axis oriented, with atomically smooth surfaces. However, the film…
Scalable fabrication of magnetic 2D materials and heterostructures constitutes a crucial step for scaling down current spintronic devices and the development of novel spintronic applications. Here, we report on van der Waals (vdW) epitaxy of the layered magnetic metal Fe$_3$GeTe$_2$ - a 2D crystal with highly tunable properties and a high prospect for room temperature ferromagnetism - directly on graphene by employing molecular beam epitaxy. Morphological and structural characterization confirmed the realization of large-area, continuous Fe$_3$GeTe$_2$/graphene heterostructure films with stabl…
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 …
Angle-resolved photoemission spectroscopy (ARPES) is the key momentum-resolved technique for direct probing of the electronic structure of a material. However, since it is very surface-sensitive, it has been applied to a relatively small set of complex oxides that can be easily cleaved in ultra-high vacuum. Here we describe a new multi-module system at Brookhaven National Laboratory (BNL) in which an oxide molecular beam epitaxy (OMBE) is interconnected with an ARPES and a spectroscopic-imaging scanning tunneling microscopy (SI-STM) module. This new capability largely expands the range of comp…
The remote epitaxy was originally proposed to grow a film, which is not in contact but crystallographically aligned with a substrate and easily detachable due to a van der Waals material as a space layer. Here we show that the claimed remote epitaxy is more likely to be nonremote `thru-hole' epitaxy. On a substrate with thick and symmetrically incompatible van der Waals space layer or even with a three-dimensional amorphous oxide film in-between, we demonstratively grew GaN domains through thru-holes via connectedness-initiated epitaxial lateral overgrowth, not only readily detachable but also…
The exploration of emerging materials physics and prospective applications of two-dimensional materials greatly relies on the growth control of their thickness, phases, morphologies and film-substrate interactions. Though substantial progresses have been made for the development of two-dimensional films from conventional layered bulky materials, particular challenges remain on obtaining ultrathin, single crystalline, dislocation-free films from intrinsically non-Van der Waals-type three-dimensional materials. In this report, with the successful demonstration of single crystalline ultrathin lar…
We show that reflection high-energy electron diffraction (RHEED) can be used as a highly sensitive tool to track surface and resulting film stoichiometry in adsorption-limited molecular beam epitaxy of (001) SrTiO3 thin films. Even under growth conditions that yield films with a lattice parameter that is identical to that of stoichiometric bulk crystals within the detection limit of high-resolution x-ray diffraction (XRD), changes in surface reconstruction occur from (1x1) to (2x1) to c(4x4) as the equivalent beam pressure of the Ti metalorganic source is increased. These surface reconstructio…
We demonstrate selective area epitaxy of GaAs films using patterned graphene masks on a Ge (001) substrate. The GaAs selectively grows on exposed regions of the Ge substrate, for graphene spacings as large as 10 microns. The selectivity is highly dependent on the growth temperature and annealing time, which we explain in terms of temperature dependent sticking coefficients and surface diffusion. The high nucleation selectivity over several microns sets constraints on experimental realizations of remote epitaxy.
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）
