While the growth of germanene has been claimed on many substrates, the exact crystal structures remain controversial. Here, we systematically explore the possible structures formed by Ge deposition onto Al(111) surface by combining density-functional theory (DFT) and global optimization algorithm. We show that, by high-level random-phase approximation (RPA) calculations, the formation of germanene on Al(111) is energetically unfavorable with positive formation energy. The two experimental phases are identified as honeycomb alloys Al3Ge3/Al(111)(r7xr7) and Al3Ge4/Al(111)(3x3), by combining ab initio evolutionary simulations, RPA calculations, and available experimental data from scanning tunneling microscopy (STM) and low-energy electron diffraction (LEED). Al3Ge4/Al(111)(3x3) is an interesting structure with a vacancy in the substrate, which accounts for the dark clover pattern in the experimental STM image. Our results clarify the structural controversy of the Ge/Al(111) system and indicate the fabrication of germanene may remain challenging.
Unlike silicene, for which the demonstration of its existence has been done through numerous independent studies, the possibility of growing epitaxial germanene remains highly controversial. It has been recently shown by scanning tunneling microscopy that the (3 x 3) surface reconstruction formed upon Ge deposition on Al(111) presents a honeycomb structure, and it was assigned to a pure germanene monolayer. Using quantitative measurements by surface X-ray diffraction compared to density functional theory calculations, we demonstrate that this Ge/Al(111) (3 x 3) reconstruction corresponds, in f…
Theoretical studies have shown that new physical properties such as tunable gap openings or quantum spinHall effects could be expected from group-IV graphene analogs (silicene, germanene, stanene). While therehave been numerous studies of growth of such Si, Ge, Sn monolayers, the demonstration of their hexagonalorganization has been often based on postgrowth characterization, and their analogy to graphene has remainedcontroversial. Our real-time scanning tunneling microscopy (STM) observation during Ge deposition on Ag(111)in the 380--430 K temperature range reveals that Ag atoms are involved …
Germanene, a two-dimensional honeycomb germanium crystal, is grown at graphene/Ag(111) and hexagonal boron nitride (h-BN)/Ag(111) interfaces by segregating germanium atoms. A simple annealing process in N2 or H2/Ar at ambient pressure leads to the formation of germanene, indicating that an ultrahigh-vacuum condition is not necessary. The grown germanene is stable in air and uniform over the entire area covered with a van der Waals (vdW) material. As an important finding, it is necessary to use a vdW material as a cap layer for the present germanene growth method since the use of an Al2O3 cap l…
Germanene, a graphene like single layer structure of Ge, has been shown to be stable and recently grown on Pt and Au substrates. We show that a Ge adatom adsorbed to germanene pushes down the host Ge atom underneath and forms a dumbbell structure. This exothermic process occurs spontaneously. The attractive dumbbell-dumbbell interaction favors high coverage of dumbbells. This letter heralds stable new phases of germanene, which are constructed from periodically repeating coverage of dumbbell structures and display diversity of electronic and magnetic properties.
Two-dimensional (2D) honeycomb lattices beyond graphene, such as germanene, promise new physical properties such as quantum spin Hall effect. While there have been many claims of growth of germanene, the lack of precise structural characterization of the epitaxial layers synthesized hinders further research. The striped layer formed by Ge deposition on Ag(111) has been recently ascribed as a stretched germanene layer. Using surface X-ray diffraction and density functional theory calculations, we demonstrate that it corresponds in fact to a Ag$_2$Ge surface alloy with an atomic density 6.45% hi…
We report on a systematic comparative study of the spin Hall efficiency between highly face-centered cubic (fcc)-textured Pt-Al alloy films grown on MgO(001) and poorly-crystallized Pt-Al alloy films grown on SiO$_2$. Using CoFeB as the detector, we show that for Al compositions centering around $x = 25$, mainly L1$_{2}$ ordered Pt$_{100-x}$Al$_x$ alloy films grown on MgO exhibit outstanding charge-spin conversion efficiency. For Pt$_{78}$Al$_{22}$/CoFeB bilayer on MgO, we obtain damping-like spin Hall efficiency as high as $ξ_\textrm{DL} \sim +0.20$ and expect up to seven-fold reduction of po…
Using a gold (111) surface as a substrate we have grown in situ by molecular beam epitaxy an atom-thin, ordered, two-dimensional multi-phase film. Its growth bears strong similarity with the formation of silicene layers on silver (111) templates. One of the phases, forming large domains, as observed in Scanning Tunneling Microscopy, shows a clear, nearly flat, honeycomb structure. Thanks to thorough synchrotron radiation core-level spectroscopy measurements and advanced Density Functional Theory calculations we can identify it to a $\sqrt{3}$x$\sqrt{3}$R(30°) germanene layer in coincidence wit…
For the study of ferromagnetic materials which are compatible with group-IV semiconductor spintronics, we demonstrate control of the ferromagnetic properties of Heusler-alloys Fe_3-xMn_xSi epitaxially grown on Ge(111) by tuning the Mn composition x. Interestingly, we obtain L2_1-ordered structures even for nonstoichiometric atomic compositions. The Curie temperature of the epilayers with x ~ 0.6 exceeds 300 K. Theoretical calculations indicate that the electronic structures of the nonstoichiometric Fe_3-xMn_xSi alloys become half-metallic for 0.75 < x < 1.5. We discuss the possibility of room-…
Half-Heusler alloy topological semimetal YPtBi is a promising candidate for an efficient spin source material having both large spin Hall angle $θ$$_{SH}$ and high thermal stability. However, high-quality YPtBi thin films with low bulk carrier density are usually grown at 600$°$C, which exceeds the limitation of 400$°$C for back end of line (BEOL) process. Here, we investigate the crystallinity and spin Hall effect of YPtBi thin films grown at lower growth temperature down to 300$°$C. Although $θ$$_{SH}$ degraded with lowering the growth temperature to 300$°$C due to degradation of the crystal…
Inverse Heusler alloy Mn2CoAl thin films, known as a spin-gapless semiconductor (SGS), grown by three different methods: ultra-high vacuum magnetron spattering, Ar-ion beam assisted sputtering, and molecular beam epitaxy, are investigated by comparing their electric transport properties, microstructures and atomic-level structures. Of the samples, the Mn2CoAl thin film grown by MBE consists of Mn- and Co-rich phases, the structures of which are determined to be the L21B-type and disordered L21-type, respectively, according to anomalous XRD analysis. None of them forms the XA-type structure exp…
As a continuation of work on metal and alloy "plants" synthesis on porous membranes by means of pulsed current electroplating volume metallic microstructures resembling such natural objects as shells, cabbage leaves, mushrooms are grown and presented in their modest elegance. Such structures are formed from PdNi and PdCo alloys as well as Ag, Cu and Ni in conditions defined by the shape of membrane pores and the parameters of the pulsed current. It is shown that the obtained complex structures are formed by layers of metallic nanowires as a result of their self-assembly while growing during th…
New perspective cubic quasi-alloys CdO/MgO short period superlattices were grown on sapphire substrates by plasma assisted molecular beam epitaxy. Their crystal quality was characterized using High Resolution X-ray Diffraction (HRXRD) and Transmission Electron Microscopy (TEM) techniques. The thickness and growth rate of MgO and CdO individual layers have been extracted. Small angle X-ray diffraction peaks corresponding to the period of the superlattices ranging from 0.6 to 5 nm were clearly observed. From the XRD measurements we obtain 65% relaxation to the substrate of superlattice (SL) in S…
Inspired by the unique properties of graphene, the focus in the literature is now on investigations of various two-dimensional (2D) materials with the aim to explore their properties for future applications. The group IV analogues of graphene, i.e., silicene, germanene and stanene have been intensively studied in recent years. However, their semi-metallic band structures hamper their use in electronic applications. Hence, the synthesis of 2D materials with band gaps of various sizes has attracted a large interest. Here, we report a successful preparation of a 2D Te-Ag binary alloy with a honey…
A large and ideal Rashba-type spin-orbit splitting is desired for the applications of materials in spintronic devices and the detection of Majorana Fermions in solids. Here, we propose an approach to achieve giant and ideal spin-orbit splittings through a combination of ordered surface alloying and interface engineering, that is, growing alloy monolayers on an insulating polar surface. We illustrate this unique strategy by means of first-principles calculations of buckled hexagonal monolayers of SbBi and PbBi supported on Al$_2$O$_3$(0001). Both systems display ideal Rashba-type states with gi…
Alloying enables engineering of the electronic structure of semiconductors for optoelectronic applications. Due to their similar lattice parameters, the two-dimensional semiconducting transition metal dichalcogenides of the MoWSeS group (MX2 where M= Mo or W and X=S or Se) can be grown as high-quality materials with low defect concentrations. Here we investigate the atomic and electronic structure of Mo(1-x)WxS2 alloys using a combination of high-resolution experimental techniques and simulations. Analysis of the Mo and W atomic positions in these alloys, grown by chemical vapour transport, sh…
Unlike other II-VI semiconductors, CdO-based transparent oxide has great potential application for the fabrication of many optoelectronic devices. In this work, we study the growth of CdxMg1-xO alloys on m- and on c-plane sapphire substrates in Cd-rich to Mg-rich conditions using the plasma-assisted molecular beam epitaxy method. A structural and morphological study of CdMgO random alloys was carried out using X-ray diffraction and Atomic Force Microscope (AFM) techniques whereas composition analysis was done by Energy-dispersive X-ray (EDX) spectroscopy method. The optical properties of thin …
We have grown a single crystal of the equiatomic FeCoCrMnAl high-entropy alloy. The crystal was grown by means of the Bridgman technique and is about 1 cm in diameter and 6.6 cm in length. X-ray Laue images taken at various positions on the surface are sharp and mutually consistent, reflecting its single-crystal nature. We thus report on the first successful growth of a single crystal of a high-entropy alloy with a volume of the order of cubic centimeters. The material has a microstructure consisting of B2 inclusions in a body-centered cubic matrix on the 10 nm length scale.
The authors demonstrated that a full-Heusler Co2FeGe (CFG) alloy thin film was epitaxially grown by rapid-thermal-annealing-induced germanidation of an Fe/Co/pseudo-Ge(001)-on-insulator (GOI) multilayer formed on a Si-on-insulator (SOI) substrate. X-ray diffraction (XRD) measurements with the out-of-plane and in-plane configurations revealed that the CFG film was epitaxially grown along the [001] direction with the in-plane epitaxial relation of CFG[100]||GOI[100], although the film slightly contained a texture component. The strong (111) and (200) superlattice diffraction intensities indicate…
Over the years attempts have been made to compensate for the inherent weaknesses in the bulk state of the multiferroic BiFeO3, such as high leakage current and the absence of ferromagnetic correlation, and exploit its magnetoelectric potential by forming solid solutions with other perovskites. Studies in the recent few years have shown that alloying of BiFeO3 with BaTiO3, both with and without additives, can induce both ferroelectric and ferromagnetic switching. While the coexistence of both the ferroic orders is encouraging from the view point of technological applications, the origin of ferr…
Poly- and single-crystal thin films of U-Mo alloys have been grown both on glass and sapphire substrates by UHV magnetron sputtering. X-ray and Electron Backscatter Diffraction data indicate that for single-crystal U1-xMox alloys, the pure cubic uranium gamma-phase exists for x > 0.22 (10 wt.% Mo). Below 10 wt.% Mo concentration, the resulting thin film alloys exhibited a mixed alpha-gamma uranium phase composition.
We report on the synthesis of carbon nanotubes on quasicrystalline alloys. Aligned multiwalled carbon nanotubes (MWNTs) on the conducting faces of decagonal quasicrystals were synthesized using floating catalyst chemical vapor deposition. The alignment of the nanotubes was found perpendicular to the decagonal faces of the quasicrystals. A comparison between the growth and tube quality has also been made between tubes grown on various quasicrystalline and SiO2 substrates. While a significant MWNT growth was observed on decagonal quasicrystalline substrate, there was no significant growth observ…
The alpha/beta interface in Ti-6Al-2Sn-4Zr-6Mo (Ti-6246) is investigated via centre of symmetry analysis, both as-grown and after 10% cold work. Semi-coherent interface steps are observed at a spacing of 4.5 +/-1.13 atoms in the as-grown condition, in good agreement with theory prediction (4.37 atoms). Lattice accommodation is observed, with elongation along [-1 2 -1 0]alpha and contraction along [1 0 -1 0]alpha . Deformed alpha exhibited larger, less coherent steps with slip bands lying in {110}beta. This indicates dislocation pile-up at the grain boundary, a precursor to globularisation, off…
$\text{Ge}_{1-y}\text{Sn}_y$ alloys with compositions in the 0.15 < $y$ < 0.30 range have been grown directly on Si substrates using a chemical vapor deposition approach that allows for growth temperatures as high as 290 $^{\circ}$C. The films show structural properties that are consistent with results from earlier materials with much lower Sn concentrations. These include the lattice parameter and the Ge-Ge Raman frequency, which are found to depend linearly on composition. The simplicity of the structures, directly grown on Si, makes it possible to carry out detailed optical studies. Sharp a…
Despite many efforts the origin of a ferromagnetic (FM) response in ZnMnO and ZnCoO is still not clear. Magnetic investigations of our samples, not discussed here, show that the room temperature FM response is observed only in alloys with a non-uniform Mn or Co distribution. Thus, the control of their distribution is crucial for explanation of contradicted magnetic properties of ZnCoO and ZnMnO reported till now. In the present review we discuss advantages of the Atomic Layer Deposition (ALD) growth method, which enables us to control uniformity of ZnMnO and ZnCoO alloys. Properties of ZnO, Zn…
Solid solubility (SS) is one of the most important features of alloys, which is usually difficult to be largely tuned in the entire alloy concentrations by external approaches. Some alloys that were supposed to have promising physical properties could turn out to be much less useful because of their poor SS, e.g., the case for monolayer BNC [(BN)1-x(C2)x] alloys. Until now, an effective approach on significantly enhancing SS of (BN)1-x(C2)x in the entire x is still lacking. In this article, a novel mechanism of selective orbital coupling between high energy wrong-bond states and surface states…
Hf silicate films (HfO_2)_{0.25}(SiO_2)_{0.75} with thicknesses in the range 4-20 nm were grown on silicon substrate by atomic layer deposition at 350 deg.C.The Hf distributions in as-grown and 800 deg.C annealed films were investigated by high resolution transmission electron microscopy (HRTEM), angle-resolved x-ray photoelectron spectroscopy (ARXPS) and medium energy ion scattering (MEIS). HRTEM images show a layered structure in films thinner than 8 nm. The ARXPS data also reveal a non-uniform distribution of Hf throughout the film depth. Diffusion of SiO_2 to the film surface after a longe…
Avalanche photodiodes fabricated from AlInAsSb grown as a digital alloy exhibit low excess noise. In this paper, we investigate the band structure-related mechanisms that influence impact ionization. Band-structures calculated using an empirical tight-binding method and Monte Carlo simulations reveal that the mini-gaps in the conduction band do not inhibit electron impact ionization. Good agreement between the full band Monte Carlo simulations and measured noise characteristics is demonstrated.
Effect of the growth temperature and the AlN mole fraction on In incorporation and properties of quaternary III-nitride layers grown by molecular beam epitaxy
Ordered W-doped Ta2O5 nanotube arrays were grown by self-organizing electrochemical anodization of TaW alloys with different tungsten concentrations and by a suitable high temperature ammonia treatment, fully converted to W:Ta3N5 tubular structures. A main effect found is that W doping can decrease the band gap from 2 eV (bare Ta3N5) down to 1.75 eV. Ta3N5 nanotubes grown on 0.5 at% W alloy and modified with (CoOH)x as co-catalyst show ~33% higher photocurrents in photoelectrochemical (PEC) water splitting than pure Ta3N5.
HRTEM, nano-beam electronic diffraction, energy dispersive X-rays scanning spectroscopy, Vibrating Sample Magnetometry (VSM) and FerroMagnetic Resonance (FMR) techniques are used in view of comparing (static and dynamic) magnetic and structural properties of Co2MnGe (13 nm)/Al2O3 (3 nm)/Co (13 nm) tunnel magnetic junctions (TMJ), deposited on various single crystalline substrates (a-plane sapphire, MgO(100) and Si(111)). They allow for providing a correlation between these magnetic properties and the fine structure investigated at atomic scale. The Al2O3 tunnel barrier is always amorphous and …
The effects of substrate treatment, temperature and composition on the surface morphology of Ni-Cr thin films grown on MgO(001) are studied by scanning tunneling microscopy (STM) and atomic force microscopy (AFM). A combination of acid-etching and high temperature deposition (400C) will result in smooth films and terraces (up to 30 nm wide) suitable for the study of progression of chemical reactions on the surface. Two different treatments are used to prepare the MgO substrates for deposition and they introduce characteristic differences in film surface morphology. Thin films that are grown on…
We report on silicon delta doping of metalorganic vapor-phase epitaxy-grown \b{eta}-Ga2O3 thin films using silane precursor. Delta-doped \b{eta}-Ga2O3 epitaxial films are characterized using capacitance-voltage profiling and secondary-ion mass spectroscopy. Electron sheet charge density in the range of 2.9e12 cm-2 to 8e12 cm-2 with a half width at half maximum ranging from 6.2 nm to 3.5 nm is measured. We also demonstrate a high density (6.4e12 cm-2) degenerate two-dimensional electron gas using a delta-doped \b{eta}-(Al0.26Ga0.74)2O3/\b{eta}-Ga2O3 heterostructure.The total charge could also i…
A method of growing mushroom or shell like nanostructured metal convex concave models has been worked out. Silver,copper,nickel,rhodium and Pd-Ni,Pd-Co alloy structures are reproduced as a result of self-assembly of nanowires growing on porous membranes in the course of pulse current electrodeposition. It is shown that the method allows to model not only the shell shape but also the hierarchical structure at the nano, micro and mesolevels. A 1,2 mm sized shell was grown from Pd-Ni alloy. The architecture of the models was studied by fragmentation and chemical etching. The images were obtained …
Ni2FeGa single crystals have been grown in undercooling conditions provided by a glass-purification method. It has been found that trace amounts of gamma phase embededin the single crystalline matrix preferentially orients in the <100> orientation along the growth direction. This gamma phase generates directional residual stress and results in an anisotropic two-way shape memory effect. Large strains of -2.5% in the [001] and 1.5% in the [010] directions have been observed. This trace gamma phase also improves the ductility of the material and thus the crystals could be plastically deformed at…
The ability to protect refined metals from reactive environments is vital to many industrial and academic applications. Current solutions, however, typically introduce several negative effects, including increased thickness and changes in the metal physical properties. In this paper, we demonstrate for the first time the ability of graphene films grown by chemical vapor deposition to protect the surface of the metallic growth substrates of Cu and Cu/Ni alloy from air oxidation. SEM, Raman spectroscopy, and XPS studies show that the metal surface is well protected from oxidation even after heat…
We discuss the possibility of a 2D ordered structure formed upon deposition of Si on metal surfaces. We investigate the atomic and electronic structure of the Si-$(\sqrt{19}\times\sqrt{19})R23.4^{\circ}$/Pt(111) surface reconstruction by means of a set of experimental surface-science techniques supported by theoretical calculations. The theory achieves a very good agreement with the experimental results and corroborate beyond any doubt that this phase is a surface alloy consisting of Si$_3$Pt tetramers that resembles a twisted Kagome lattice. These findings render unlikely any formation of sil…
We have analyzed by means of scanning tunneling microscopy and spectroscopy the atomic and electronic structure of monolayers of 1T-VxPt1-xSe2 alloys grown by molecular beam epitaxy on epitaxial graphene substrates. We have focused on the composition range (0.1<x<0.35) where ferromagnetic behaviour has recently been demonstrated. For low Pt concentration, (x=0.07 and x=0.21), small domains (a few nanometres in diameter) exhibiting the characteristic superstructure of the charge density wave (CDW) state of pristine VSe2 monolayer remain visible on most of the sample surface. Thus alloying prese…
Pulsed Laser Deposition allows to obtain W and W-Ta alloy coatings with different nanostructures, monitored by X-ray diffraction. The correlation between such structures and the elastic properties is investigated for amorphous-like, ultra-nano- and nano-crystalline coatings obtained by tuning the gas pressure during deposition, annealing temperature and Ta concentration. The full elastic characterization is achieved by surface Brillouin spectroscopy, interpreted by isotropic and anisotropic film models. Amorphous like coatings are obtained with He pressures of tens of Pa. In comparison with bu…
Mn$_2$VAl Heusler alloy films were epitaxially grown on MgO(100) single crystal substrates by means of ultra-high-vacuum magnetron sputtering. A2 and L2$_1$ type Mn$_2$VAl order was controlled by the deposition temperatures. A2-type Mn$_2$VAl films showed no spontaneous magnetization and L2$_1$-type Mn$_2$VAl films showed ferrimagnetic behavior with a maximum saturation magnetization of 220 emu/cm$^3$ at room temperature. An antiferromagnetic reflection was observed with neutron diffraction at room temperature for an A2-type Mn$_2$VAl film deposited at 400$^\circ$C. A bilayer sample of the ant…
Polycrystalline diamond coatings have been grown on cemented carbide substrates with different aspect ratios by a microwave plasma CVD in methane-hydrogen gas mixtures. To protect the edges of the substrates from non-uniform heating due to the plasma edge effect, a special plateholder with pockets for group growth has been used. The difference in heights of the substrates and plateholder, and its influence on the diamond film mean grain size, growth rate, phase composition and stress was investigated. The substrate temperature range, within which uniform diamond films are produced with good ad…
Compound semiconductor alloys of the type ABC find widespread applications as their electronic bulk band gap varies continuously with x, and therefore a tayloring of the energy gap is possible by variation of the concentration. We model the electronic properties of such semiconductor alloys by a multiband tight-binding model on a finite ensemble of supercells and determine the band gap of the alloy. This treatment allows for an intrinsic reproduction of band bowing effects as a function of the concentration x and is exact in the alloy-induced disorder. In the present paper, we concentrate on b…
