(111)NiO epitaxial layers are grown on c-sapphire substrates by pulsed laser deposition (PLD) technique. Structural and morphological properties of the films are studied using in-plane as well as out-of-plane high resolution X-ray diffraction and atomic force microscopy techniques as functions of growth temperature, oxygen pressure and the pulses count of the laser. The study shows that continuous epitaxial films of thickness as low as 3 nm with high crystalline quality, smooth surface and interface morphology can be grown by this technique. The study also reveals the co-existence of 60°-rotated (111) triangular domains of NiO in the film. The study also evidences the presence of a very low density of 60-degree dislocations in these films. Density of screw and edge dislocations are also estimated to be quite low. It has been found that growth-temperature, oxygen partial pressure and the film thickness can influence differently the density of various dislocation types. These parameters are also found to affect significantly the strain developed in the films.
In their recent publication, Zhao et al. [J. Appl. Phys. 110, 033523 (2011)] claim to have found a new three-dimensional relationship for niobium-on-sapphire epitaxy. However, two critical errors were made in the analysis of x-ray diffraction measurements. The crystal structure of sapphire (alpha-Al2O3) was erroneously cited as hexagonal close-packed, and crystallographic orientations of sapphire were misidentified. Correcting these errors, one finds their claim unjustified.
This paper reports on the epitaxial growth of hexagonal boron nitride (hBN) films on sapphire substrates in a cold wall chemical vapor deposition (CVD) system where different sapphire nitridation and hBN growth temperatures were employed. A thin and amorphous nitridated layer was formed at a low temperature (850 C), which enabled subsequent epitaxial hBN growth at 1350 C. The influences of the sapphire nitridation temperature and the growth temperature on the film quality were analyzed by X-ray diffraction (XRD) measurements. Higher than optimum nitridation and growth temperatures improve the …
In this article, we estimate hydrostatic stress developed in gallium ion implanted gallium nitride epitaxial layers using Raman measurements. We have calculated deformation potential constants for $E_2$(high) mode in these epi-layers. The presence of a polar phonon-plasmon coupling in these systems has also been demonstrated. In as-implanted samples, with an increase in implantation fluence, we have observed disorder-activated Raman scattering.
Uniform single layer graphene was grown on single-crystal Ir films a few nanometers thick which were prepared by pulsed laser deposition on sapphire wafers. These graphene layers have a single crystallographic orientation and a very low density of defects, as shown by diffraction, scanning tunnelling microscopy, and Raman spectroscopy. Their structural quality is as high as that of graphene produced on Ir bulk single crystals, i.e. much higher than on metal thin films used so far.
Magnetic tunnel junctions (MTJ) have been grown by using molecular beam epitaxy on c-plane Al2O3 substrates. The MTJ stacks consist of two ferromagnetic hcp-Co layers separated by a thin insulating h-BN barrier. The samples have been grown in a single run revealing single crystalline epitaxial structures with sharp interfaces as observed by applying transmission electron microscopy. The in-plane magnetization experiments have revealed separate magnetization switching of a thin top Co (soft) layer and a thick bottom Co (hard) layer. At zero magnetic field the two Co layers are found in an antip…
We use ultra-high vacuum chemical vapor deposition to grow polycrystalline silicon carbide (SiC) on c-plane sapphire wafers which are then annealed between 1250 and 1450°C in vacuum to create epitaxial multilayer graphene (MLG). Despite the surface roughness and small domain size of the polycrystalline SiC, a conformal MLG film is formed. By planarizing the SiC prior to graphene growth, a reduction of the Raman defect band is observed in the final MLG. The graphene formed on polished SiC films also demonstrates significantly more ordered layer-by-layer growth and increased carrier mobility for…
We report on the generation and transport of thermal spin currents in fully epitaxial γ-Fe$_2$O$_3$/NiO(001)/Pt and Fe$_3$O$_4$/NiO(001)/Pt trilayers. A thermal gradient, perpendicular to the plane of the sample, generates a magnonic spin current in the ferrimagnetic maghemite (γ-Fe$_2$O$_3$) and magnetite (Fe$_3$O$_4$) thin films by means of the spin Seebeck effect. The spin current propagates across the epitaxial, antiferromagnetic insulating NiO layer, before being detected in the Pt layer by the inverse spin Hall effect. The transport of the spin signal is studied as a function of the NiO …
We report the results of x-ray scattering studies of AlN on c-plane sapphire during reactive radiofrequency magnetron sputtering. The sensitivity of in situ x-ray measurements allowed us to follow the structural evolution of strain and roughness from initial nucleation layers to fullyrelaxed AlN films. A growth rate transient was observed, consistent with the initial formation of non-coalesced islands with significant oxygen incorporation from the substrate. Following island coalescence, a steady state growth rate was seen with a continuous shift of the c and a lattice parameters towards the r…
We report epitaxial growth and characterization of GaN thin films on sapphire (0001) substrates using low temperature GaN intermediate layer by plasma assisted molecular beam epitaxy (PA-MBE) technique. As grown and annealed GaN thin films were studied by high- resolution X-ray diffraction (HRXRD), atomic force microscopy (AFM), Hall Effect and photoluminescence (PL). It has been found that there is a significant improvement in the quality of the GaN films after annealing at 725 \degree C in terms of electron mobility, full width at half maximum (FWHM) of omega (ω) scan around (0002) XRD peak …
(001) oriented NiO/NiFe bilayers were grown on single crystal MgO (001) substrates by ion beam sputtering in order to determine the effect that the crystalline orientation of the NiO antiferromagnetic layer has on the magnetization curve of the NiFe ferromagnetic layer. Simple models predict no exchange anisotropy for the (001)-oriented surface, which in its bulk termination is magnetically compensated. Nonetheless exchange anisotropy is present in the epitaxial films, although it is approximately half as large as in polycrystalline films that were grown simultaneously. Experiments show that d…
Realization of wafer-scale single-crystal films of transition metal dichalcogenides (TMDs) such as tungsten sulfide requires epitaxial growth and coalescence of oriented domains to form a continuous monolayer. The domains must be oriented in the same crystallographic direction on the substrate to avoid the formation of metallic inversion domain boundaries (IDBs) which are a common feature of layered chalcogenides. Here we demonstrate fully-coalesced single orientation tungsten sulfide monolayers on 2-inch diameter c-plane sapphire by metalorganic chemical vapor deposition using a multi-step gr…
Molecular-beam epitaxy (MBE) provides a simple but powerful way to synthesize large-area high-quality thin films and heterostructures of a wide variety of materials including accomplished group III-V and II-VI semiconductors as well as newly-developing oxides and chalcogenides, leading to major discoveries in condensed-matter physics. For two-dimensional (2D) materials, however, main fabrication routes have been mechanical exfoliation and chemical-vapor deposition by making good use of weak van der Waals bonding nature between neighboring layers, and MBE growth of 2D materials, in particular o…
The epitaxy of MoO2 on c_plane sapphire substrates is examined. A theoretical approach, based on density functional theory calculations of the strain energy, allowed to predict the preferred layer/substrate epitaxial relationships. To test the results of these calculations, MoO2/(001) Al2O3 heterostructures were grown using the chemically_driven isothermal close space vapour transport technique. At the early stages of the growth, two kinds of morphologies were obtained, using the same growth parameters: lying and standing flakes. The composition and morphology, as well as the layer/substrate e…
Raman spectroscopy is utilized to study the magnetic characteristics of heteroepitaxial NiO thin films grown by plasma-assisted molecular beam epitaxy on MgO(100) substrates. For the determination of the Néel temperature, we demonstrate a reliable approach by analyzing the temperature dependence of the Raman peak originating from second-order scattering by magnons. The antiferromagnetic coupling strength is found to be strongly influenced by the growth conditions. The low-temperature magnon frequency and the Néel temperature are demonstrated to depend on the biaxial lattice strain and the degr…
We prepare the high quality epitaxial MgO(001)[100]/Pt(001)[100]/NiO(001)[100]/FeNi/SiO2 films to investigate the spin transport in the NiO antiferromagnetic insulator. The ferromagnetic resonance measurements of the FeNi under a spin current injection from the Pt by the spin Hall effect revealed the change of the ferromagnetic resonance linewidth depending on the amount of the spin current injection. The results can be interpreted that there is an angular momentum transfer through the NiO. A high efficient angular momentum transfer we observed in the epitaxial NiO can be attributed to the wel…
Zero field cooled spontaneous exchange bias (SEB) is observed in epitaxial La0.7Sr0.3MnO3 (LSMO):NiO self-assembled nanocomposite thin films grown on (001) SrTiO3 single crystal substrate by pulsed laser deposition. SEB is displayed by the novel asymmetry in the hysteresis loop of the composite film along with the field cooled conventional exchange bias (CEB) effect. The training effect shows that exchange bias relaxation is disorder mediated. It is revealed from DC magnetization results that such nanocomposite film divulges spin glass like behaviour, which is arising due to competing ferromag…
We present results on growth of large area epitaxial ReS2 thin film both on c plane sapphire substrate and MoS2 template by pulsed laser deposition (PLD). Films tend to grow with (0001) ReS2 perpendicular to (0001) Al2O3 and (0001) ReS2 perpendicular to (0001) MoS2 parallel to (0001) Al2O3 at deposition temperature below 300 deg C. Films are polycrystalline grown at temperature above 300 deg C. The smoothness and quality of the films are significantly improved when grown on MoS2 template compared to sapphire substrate. The results show that PLD is suitable to grow ReS2 epitaxial thin film over…
This letter describes a new inorganic shadow mask that has been employed for the evaporation of all-epitaxial Al/Al2O3/Al superconducting tunnel junctions. Organic resists that are commonly used for shadow masks and other lift-off processes are not compatible with ultra-high vacuum deposition systems, and they can break down at even moderately elevated temperatures. The inorganic mask described herein does not suffer these same shortcomings. It was fabricated from a Ge/Nb bilayer, comprising suspended Nb bridges supported by an undercut Ge sacrificial layer. Utilizing such a bilayer mask on C-…
NbN films are grown on c-plane sapphire substrates by molecular beam epitaxy. The structural and superconducting properties of the film are characterized to demonstrate that growth parameters such as substrate temperature and active nitrogen flux effect the structural phase of films, and thereby the superconducting critical temperature. Four phases of NbN are identified for films grown in different conditions. In a novel finding, we demonstrate that atomically flat and highly crystalline $β$-$\textrm{Nb}_2\textrm{N}$ films can be grown at substrate temperatures of 1100 \degree C or higher, and…
Gallium oxide epitaxial layers grown on native substrates and basal plane sapphire were characherized by X-ray phtotelectron and optical reflectance spectroscopies. The XPS electronic structure mapping was coupled to Density functional theory calculations.
We report the observation of the three-dimensional angular dependence of the spin Hall magnetoresistance (SMR) in a bilayer of the epitaxial antiferromagnetic insulator NiO(001) and the heavy metal Pt, without any ferromagnetic element. The detected angular-dependent longitudinal and transverse magnetoresistances are measured by rotating the sample in magnetic fields up to 11 T, along three orthogonal planes (xy-, yz- and xz-rotation planes, where the z-axis is orthogonal to the sample plane). The total magnetoresistance has contributions arising from both the SMR and ordinary magnetoresistanc…
Epitaxial growth and controllable doping of wafer-scale single-crystal transition-metal dichalcogenides (TMDCs) are two central tasks for extending Moore's law beyond silicon. However, despite considerable efforts, addressing such crucial issues simultaneously under two-dimensional (2D) confinement is yet to be realized. Here we design an ingenious epitaxial strategy to synthesize record-breaking 4-inch single-crystal Fe-doped TMDCs monolayers on industry-compatible c-plane sapphire without miscut angle. In-depth characterizations and theoretical calculations reveal that the introduction of Fe…
Single crystal metal films on insulating substrates are attractive for microelectronics and other applications, but they are difficult to achieve on macroscopic length scales. The conventional approach to obtaining such films is epitaxial growth at high temperature using slow deposition in ultrahigh vacuum conditions. Here we describe a different approach: sputter deposition at modest temperatures followed by annealing to induce secondary grain growth. We show that polycrystalline as-deposited Cu on α-Al2O3(0001) can be transformed into Cu(111) with centimeter-sized grains. Employing optical m…
We study the underlying chemical, electronic and magnetic properties of a number of magnetite based thin films. The main focus is placed onto NiO/Fe$_3$O$_4$(001) bilayers grown on MgO(001) and Nb-SrTiO$_3$(001) substrates. We compare the results with those obtained on pure Fe$_3$O$_4$(001) thin films. It is found that the magnetite layers are oxidized and Fe$^{3+}$ dominates at the surfaces due to maghemite ($γ$-Fe$_2$O$_3$) formation, which decreases with increasing magnetite layer thickness. From a layer thickness of around 20 nm on the cationic distribution is close to that of stoichiometr…
We have successfully grown epitaxial La$_{1.67}$Sr$_{0.33}$NiO$_4$ films with a small crystalline mosaic using pulsed laser deposition. With synchrotron radiation, the x-ray diffraction peaks associated with charge stripes have been successfully observed for relatively thick films. Anomalies due to the charge-ordering transition have been examined using four-point probe resistivity measurements. X-ray scattering provides direct evidence for suppression of the stripe phase in thin samples; the phase disappears for film thicknesses $\leqslant$ 2600 ~Å. The suppression appears to be a result of s…
Heteroepitaxial growth of selected group IV-VI nitrides on various orientations of sapphire (α-Al2O3) is demonstrated using atomic layer deposition. High quality, epitaxial films are produced at significantly lower temperatures than required by conventional deposition methods. Characterization of electrical and superconducting properties of epitaxial films reveals a reduced room temperature resistivity and increased residual resistance ratio (RRR) for films deposited on sapphire compared to polycrystalline samples deposited concurrently on fused quartz substrates.
Spot Profile Analysis Low Energy Electron Diffraction of Plasma-Enhanced Chemical Vapor Deposition Grown Epitaxial Few-Layer Graphene on Sapphire
University of Duisburg-Essen（杜伊斯堡-埃森大学）；Faculty of Engineering, University of Duisburg-Essen（杜伊斯堡-埃森大学工程学院）；Department of Chemistry and Waterloo Institute for Nanotechnology（化学系与滑铁卢纳米技术研究所）；Center for Nanointegration (CENIDE)（纳米集成中心）
Epitaxial Al/GaAs/Al structures having controlled thickness of high-quality GaAs and pristine interfaces have been fabricated using a wafer-bonding technique. III-V semiconductor/Al structures are grown by molecular beam epitaxy on III-V semiconductor substrates and bonded to silicon and sapphire. Selective etching is used to remove the III-V substrate followed by surface cleaning and superconductor regrowth, resulting in epitaxial Al/GaAs/Al tri-layers on sapphire or silicon substrates. Structures are characterized with reflection high energy electron diffraction, atomic force microscopy, X-r…
We report on the chemically stabilized epitaxial w-BN thin film grown on c-plane sapphire by pulsed laser deposition under slow kinetic condition. Traces of no other allotropes such as cubic (c) or hexagonal (h) BN phases are present. Sapphire substrate plays a significant role in stabilizing the metastable w-BN from h-BN target under unusual PLD growth condition involving low temperature and pressure and is explained based on density functional theory calculation. The hardness and the elastic modulus of the w-BN film are 37 & 339 GPa, respectively measured by indentation along <0001> directio…
Ultra-wide bandgap semiconductors are ushering in the next generation of high power electronics. The correct crystal orientation can make or break successful epitaxy of such semiconductors. Here it is discovered that single-crystalline layers of $α$-(AlGa)$_2$O$_3$ alloys spanning bandgaps of 5.4 - 8.6 eV can be grown by molecular beam epitaxy. The key step is found to be the use of m-plane sapphire crystal. The phase transition of the epitaxial layers from the $α$- to the narrower bandgap $β$-phase is catalyzed by the c-plane of the crystal. Because the c-plane is orthogonal to the growth fro…
Hexagonal boron nitride (hBN) has been grown on sapphire substrates by ultra-high temperature molecular beam epitaxy (MBE). A wide range of substrate temperatures and boron fluxes have been explored, revealing that high crystalline quality hBN layers are grown at high substrate temperatures, $>$1600$^\circ$C, and low boron fluxes, $\sim1\times10^{-8}$ Torr beam equivalent pressure. \emph{In-situ} reflection high energy electron diffraction (RHEED) revealed the growth of hBN layers with $60^\circ$ rotational symmetry and the $[11\bar20]$ axis of hBN parallel to the $[1\bar100]$ axis of the sapp…
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…
The current method of growing large-area graphene on Cu surfaces (polycrystalline foils and thin films) and its transfer to arbitrary substrates is technologically attractive. However, the quality of graphene can be improved significantly by growing it on single-crystal Cu surfaces. Here we show that high quality, large-area graphene can be grown on epitaxial single-crystal Cu(111) thin films on reusable basal-plane sapphire (alpha-Al2O3(0001)) substrates and then transferred to another substrate. While enabling graphene growth on Cu single-crystal surfaces, this method has the potential to av…
First principles calculations based on density functional theory are performed to investigate the structural, electronic and magnetic properties of wurtzite ZnO/NiO (0001) interface. By using DFT+U method we discover that the half-metallic behavior of wurtzite NiO (w-NiO) retains in the ZnO/NiO (0001) interface. Through analyses of density of state, charge population and magnetic moments, we find the half-metallicity is weakened around the interface but interface effect is quite localized. More over the interface system keeps a ferromagnetic ground state as bulk w-NiO does. Based on the simula…
The first epitaxial ferroelectric wurtzite film with clear polarization-electric field hysteresis behavior is presented. The coercive field of this epitaxial Al0.7Sc0.3N film on W/c-sapphire substrate is 0.4 +- 0.3 MV cm-1 (8 %) smaller than that of a conventional fiber textured film on a Pt/TiOx/SiO2/Si substrate, attributed to the 0.01 +- 0.007 Å smaller c-axis lattice parameter in the epitaxial film. The strain and decrease of the coercive field most likely originate from epitaxial strain rather than the mismatch in thermal coefficient of expansion. These results provide an insight for furt…
We use real-time spectroscopic polarimetric observations of growth and a chemical model derived therefrom, to develop a method of growing dense, two-dimensional zinc oxide epitaxially on sapphire by metalorganic chemical vapor deposition. Particulate zinc oxide formed in the gas phase is used to advantage as the deposition source. Our real-time data provide unequivocal evidence that: a seed layer is required; unwanted fractions of ZnO are deposited; but these fractions can be removed by cycling between brief periods of net deposition and etching. The transition between deposition and etching o…
The direct liquid injection chemical vapor deposition (DLI-CVD) technique has been used for the growth of cobalt ferrite (CFO) films on (100)-oriented MgAl$_2$O$_4$ (MAO) substrates. Smooth and highly epitaxial cobalt ferrite thin films, with the epitaxial relationship $\mathrm{MAO} (100)\:[001] \parallel \mathrm{CFO} (100)\:[001]$, are obtained under optimized deposition conditions. The films exhibit bulk-like structural and magnetic properties with an out-of-plane lattice constant of $8.370\;\mathrmÅ$ and a saturation magnetization of $420\;\mathrm{kA/m}$ at room temperature. The Raman spect…
We demonstrate that the highly sensitive phase-contrast properties of Bragg coherent diffraction measurements combined with the translational diversity of ptychography can provide a Bragg "dark field" imaging method capable of revealing the finger print of domain structure in metallic thin films. Experimental diffraction data was taken from a epitaxially grown niobium metallic thin film on sapphire; and analysed with the help of a careful combination of implemented refinement mechanisms.
This work presents a systematic study of stress and strain of AlxGa1-xN/AlN with composition ranging from GaN to AlN, grown on a c-plane sapphire by metal-organic chemical vapor deposition, using synchrotron radiation high-resolution X-ray diffraction and reciprocal space mapping. The c-plane of the AlxGa1-xN epitaxial layers exhibits compressive strain, while the a-plane exhibits tensile strain. The biaxial stress and strain are found to increase with increasing Al composition, although the lattice mismatch between the AlxGa1-xN and the buffer layer AlN gets smaller. A reduction in the latera…
Revealing epitaxial relationships at Ga$_2$O$_3$ interfaces with p-type oxides
Materials Science Center, National Laboratory of the Rockies（洛基山国家实验室材料科学中心）；Metallurgical and Materials Engineering Department, Colorado School of Mines（科罗拉多矿业学院冶金与材料工程系）；Renewable and Sustainable Energy Institute, University of Colorado Boulder（科罗拉多大学博尔德分校可再生与可持续能源研究所）
Several SrTiO3 (STO) thin films without electrodes processed by pulsed laser deposition, of thicknesses down to 40 nm, were studied using infrared transmission and reflection spectroscopy. The complex dielectric responses of polar phonon modes, particularly ferroelectric soft mode, in the films were determined quantitatively. The compressed epitaxial STO films on (100) La0.18Sr0.82Al0.59-Ta0.41O3 substrates (strain 0.9%) show strongly stiffened phonon responses, whereas the soft mode in polycrystalline film on (0001) sapphire substrate shows a strong broadening due to grain boundaries and/or o…
This paper reports on the growth and characterization of hexagonal boron nitride (hBN) and its use for solid-state thermal neutron detection. The hBN epilayers were grown by metalorganic chemical vapor deposition on sapphire substrates at a temperature of 1350 C. X-ray diffraction peak from the (002) hBN plane at a 2theta angle of 26.7 deg exhibited the c-lattice constant of 6.66 Å for these films. A strong peak corresponding to the high frequency Raman active mode of hBN was found for the films at 1370.5/cm. hBN-based solid-state neutron detectors were fabricated and tested with a metal-semic…
Using spin-polarized low-energy electron microscopy to study magnetization in epitaxial layered systems, we found that the area vs perimeter relationship of magnetic domains in the top Fe layers of Fe/NiO/Fe(100) structures follows a power-law distribution, with very small magnetic domain cutoff radius (about 40 nm) and domain wall thickness. This unusual magnetic microstructure can be understood as resulting from the competition between antiferromagnetic and ferromagnetic exchange interactions at the Fe/NiO interfaces, rather than from mechanisms involving the anisotropy and dipolar forces th…
