The stoichiometric "111" iron-based superconductor, LiFeAs, has attacted great research interest in recent years. For the first time, we have successfully grown LiFeAs thin film by molecular beam epitaxy (MBE) on SrTiO3(001) substrate, and studied the interfacial growth behavior by reflection high energy electron diffraction (RHEED) and low-temperature scanning tunneling microscope (LT-STM). The effects of substrate temperature and Li/Fe flux ratio were investigated. Uniform LiFeAs film as thin as 3 quintuple-layer (QL) is formed. Superconducting gap appears in LiFeAs films thicker than 4 QL at 4.7 K. When the film is thicker than 13 QL, the superconducting gap determined by the distance between coherence peaks is about 7 meV, close to the value of bulk material. The ex situ transport measurement of thick LiFeAs film shows a sharp superconducting transition around 16 K. The upper critical field, Hc2(0)=13.0 T, is estimated from the temperature dependent magnetoresistance. The precise thickness and quality control of LiFeAs film paves the road of growing similar ultrathin iron arsenide films.
We report the successful growth of tetragonal FeS film with one or two unit-cell (UC) thickness on SrTiO3(001) substrate by molecular beam epitaxy. Large lattice constant mismatch with the substrate leads to high density of defects in single UC FeS, while it has been significantly reduced in double UC thick film due to the lattice relaxation. The scanning tunneling spectra on the surface of FeS thin film reveal the electronic doping effect of single UC FeS from the substrate. In addition, at the Fermi level, the energy gaps of approximate 1.5 meV are observed in films of both thicknesses at 4.…
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…
We have carried out first-principles based DFT calculation on electronic properties of silicene monolayer on various (111) semi-conducting surfaces. We find that the relative stability and other properties of the silicene overlayer depends sensitively on whether the interacting top layer of the substrate is metal or non-metal terminated. The nature of silicene-monolayer on the metal termi- nated surface can be metallic or even magnetic, depending upon the choice of the substrate. The silicene overlayer undergoes n-type doping on metal terminated surface while it undergoes p-type doping on non …
Epitaxial layers of the topological insulator Bi2Se3 have been grown by molecular beam epitaxy on laterally lattice-matched InP(111)B substrates. High resolution X-ray diffraction shows a significant improvement of Bi2Se3 crystal quality compared to layers deposited on other substrates. The measured full width at half maximum of the rocking curve is Delta omega=13 arcsec, and the (omega-2theta) scans exhibit clear layer thickness fringes. Atomic force microscope images show triangular twin domains with sizes increasing with layer thickness. The structural quality of the domains is confirmed on…
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 …
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 epitaxial growth of {111} oriented Au on MoS$_2$ is well documented despite the large lattice mismatch (~8% biaxial strain), and the fact that a Au {001} orientation results in much less elastic strain. An analysis based on density functional and linear elasticity theories reveals that the {111} orientation is stabilized by a combination of favorable surface and interfacial contributions to the energy, and the compliance of the first layer of the MoS$_2$.
The lattice mismatch between interesting 2D materials and commonly available 3D substrates is one of the obstacles in the epitaxial growth of monolithic 2D/3D heterostructures, but a number of 2D materials have not yet been considered for epitaxy. Here we present the first molecular beam epitaxy growth of NiTe$_{2}$ 2D transition metal dichalcogenide. Importantly, the growth is realized on a nearly lattice matched GaAs(111)B substrate. Structural properties of the grown layers are investigated by electron diffraction, X-ray diffraction, and scanning tunnelling microscopy. Surface coverage and …
Epitaxial growth of BaBiO3 thin films on SrTiO3(001) and MgO(001) substrates using molecular beam epitaxy and controlling their crystal orientations competition
Antimonene is a novel two-dimensional topological semiconductor material with strain driven tunable electronic structure for future electronic and spintronic devices, but the growth of clean antimonene is not fully understood. In this work, the growth process of antimonene on silver substrate has been studied in detail by using density functional theory and particle swarm optimization algorithms. The results show that, in addition to the experimental reported flat honeycomb and $β$-phase antimonene, $α$-phase antimonene was observed to be able to grow on thus substrates, and the phases of anti…
van der Waals epitaxy of lead monoxide - PbO and application as a virtual substrate for oxide membranes
CiQUS, Centro Singular de Investigacion en Quimica Bioloxica e Materiais Moleculares, Departamento de Quimica-Fisica, Universidade de Santiago de Compostela（圣地亚哥-德孔波斯特拉大学 CiQUS 生物化学与分子材料 singular 研究中心 物理化学系）
The epitaxial growth of functional materials using a substrate with a graphene layer is a highly desirable method for improving structural quality and obtaining free-standing epitaxial nano-membranes for scientific study, applications, and economical reuse of substrates. However, the aggressive oxidizing conditions typically employed to grow epitaxial perovskite oxides can damage graphene. Here, we demonstrate a technique based on hybrid molecular beam epitaxy that does not require an independent oxygen source to achieve epitaxial growth of complex oxides without damaging the underlying graphe…
Thin crystalline layers of TaAs Weyl semimetal (9 and 18 nm thick) are grown by molecular beam epitaxy on GaAs(001) substrates. The (001) planes of the tetragonal TaAs lattice are parallel to the GaAs(001) substrate, but the corresponding in-plane crystallographic directions of the substrate and the layer are rotated by 45°. In spite of a substantial lattice mismatch (about 19%) between GaAs(001) substrate and TaAs epilayer no misfit dislocations are observed at the GaAs(001)/TaAs(001) interface. Only stacking fault defects in TaAs are detected with transmission electron microscopy. Thorough X…
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…
Mn doped GaAs thin films were grown using molecular beam epitaxy at high and low substrate temperatures. The elemental concentration depth profiles in the thin films were determined by using Auger electron spectroscopy combined with ion etching. The Mn concentration is higher near the surface and then decreases with depth for films grown at high substrate temperatures. The Mn concentration profile is much more uniform when films are grown using a low substrate temperature. What was unexpectedly found are high levels of oxygen in the low substrate temperature grown thin films.
We have performed Kinetic Monte Carlo simulation work to study the effect of diffusion anisotropy, bonding anisotropy and edge diffusion on island formation at different temperatures during the sub-monolayer film growth in Molecular Beam Epitaxy. We use simple cubic solid on solid model and event based Bortz, Kalos and Labowitch (BKL) algorithm on the Kinetic Monte Carlo method to simulate the physical phenomena. We have found that the island morphology and growth exponent are found to be influenced by substrate anisotropy as well as edge diffusion, however they do not play a significant role …
We present self-assembly of InAs/InAlAs quantum dots by droplet epitaxy technique on vicinal GaAs(111)A substrates. The small miscut angle, while maintaining the symmetries imposed to the quantum dot from the surface, allows fast growth rate thanks to the presence of preferential nucleation sites at the step edges. A 100 nm InAlAs metamorphic layer with In content > 50% is already almost fully relaxed with a very flat surface. The quantum dots emit at the 1.3 μm telecom O-band with the fine structure splitting as low as 16 μeV, thus making them suitable as photon sources in quantum communicati…
The combination of two-dimensional (2D) materials into heterostructures enabled the formation of atomically thin devices with designed properties. To achieve a high density, bottom-up integration, the growth of these 2D heterostructures via van der Waals epitaxy (vdWE) is an attractive alternative to the currently mostly employed mechanical transfer, which is still problematic in terms of scaling and reproducibility. However, controlling the location of the nuclei formation remains a key challenge in vdWE. Here, we use a focused He ion beam for a deterministic placement of defects in graphene …
A comprehensive current-voltage (I-V) characterization is performed for three different Schottky contacts; Pt, Ni and Ti, to unintentionally doped (UID) \{beta}-(Al0.19Ga0.81)2O3 grown by molecular beam epitaxy (MBE) on \{beta}-Ga2O3 for temperatures ranging between 25C -300C. Reciprocal space mapping shows the (Al0.19Ga0.81)2O3 films are strained and lattice matched to the substrate. Schottky Barrier Height (SBH), ideality factor (n), and series resistance (Rs) are extracted from the I-V characteristics for the three types of metals and temperatures. Room temperature capacitance-voltage (C-V)…
Layered van der Waals (vdW) materials grown by physical vapor deposition techniques are generally assumed to have a weak interaction with the substrate during growth. This leads to films with relatively small domains that are usually triangular and a terraced morphology. In this paper, we demonstrate that Bi2Se3, a prototypical vdW material, will form a nano-column morphology when grown on GaAs(001) substrates. This morphology is explained by a relatively strong film/substrate interaction, long adatom diffusion lengths, and a high reactive selenium flux. This discovery paves the way toward gro…
We report on the epitaxial growth and surface structure of infinite-layer cuprate Sr1-xNdxCuO2 films on SrTiO3(001) substrates by combining ozone-assisted molecular beam epitaxy and in situ scanning tunneling microscopy. Careful substrate temperature and flux control has been used to achieve single-phase, stoichiometric, and c-axis oriented films. The surface of the films is usually characterized by a mixed CuO2 surface and gridlike superstructure. The superstructure exhibits a periodicity of 3.47 nm that corresponds to a coincidence lattice between the overlayer peroxide SrO2 and underlying C…
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.
Unraveling the nature of quasi van der Waals Epitaxy of magnetic topological insulators Cr: (BixSb1-x)2Te3 on a GaAs (111) substrate through coherently strained interface
$Al_xGa_{1-x}N$ is a critical ultra-wide bandgap material for optoelectronics, but the deposition of thick, high quality epitaxial layers has been hindered by a lack of lattice-matched substrates. Here we identify the (111) face of transition metal carbides as a suitable class of materials for substrates lattice matched to (0001) $Al_xGa_{1-x}N$ and demonstrate the growth of thin film TaC which has an effective hexagonal lattice constant matched to $Al_{0.45}Ga_{0.55}N$. We explore growth conditions for sputtered TaC on sapphire substrates and investigate the effects of sputter power, layer th…
Large area epitaxy of two-dimensional (2D) layered materials with high material quality is a crucial step in realizing novel device applications based on 2D materials. In this work, we report high-quality, crystalline, large-area gallium selenide (GaSe) films grown on bulk substrates such as c-plane sapphire and gallium nitride (GaN) using a valved cracker source for Se. (002)-oriented GaSe with random in-plane orientation of domains was grown on sapphire and GaN substrates at a substrate temperature of 350-450 C with complete surface coverage and smooth surface morphology. Higher growth tempe…
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.
Three-dimensional topological insulators (3D-TIs) are a new generation of materials with insulating bulk and exotic metallic surface states that facilitate a wide variety of ground-breaking applications. However, utilization of the surface channels is often hampered by the presence of crystal defects, such as antisites, vacancies and twin domains. For terahertz device applications, twinning is shown to be highly deleterious. Previous attempts to reduce twins using technologically important InP(111) substrates have been promising, but have failed to completely suppress twin domains while preser…
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…
We have grown the ferromagnetic semiconductor GaMnAs containing up to 10% Mn by migration enhanced epitaxy at a substrate temperature of 150^oC. The alternate supply of As2 molecules and Ga and Mn atoms made it possible to grow single crystalline GaMnAs layers at very low substrate temperature, at which conventional molecular beam epitaxial growth under excess As supply is not possible due to As condensation. Secondary ion mass spectroscopy and X-ray diffraction measurements confirmed a higher Mn content in the films grown by this method in comparison to the GaMnAs layers grown by low temperat…
Mn-doped GaAs nanowires were grown in the self-catalytic growth mode on oxidized Si(100) surface by molecular beam epitaxy and characterized by scanning and transmission electron microscopy, Raman scattering, photoluminescence, cathodoluminescence, and electron transport measurements. The transmission electron microscopy studies evidenced the substantial accumulation of Mn inside the catalyzing Ga droplets at the top of the nanowires. Optical and transport measurements revealed that the limit of Mn content for self-catalysed growth of GaAs nanowires corresponds to the doping level, i.e., is mu…
Epitaxial films which contains more than one crystallographic orientation are of interest due to the possibility of altered magnetic, electrical, and optical properties. Thin films of FeSe have been grown on single-crystal MgO substrates under conditions that produces the simultaneous, epitaxial growth of tetragonal and hexagonal phases. We show that this double epitaxy is characterized by phase domains with a well-defined epitaxial relationship to each other and that the relative phase fraction can be controlled. For growth temperatures of 350-450 degrees C, the (001)-oriented tetragonal phas…
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…
Pritzker School of Molecular Engineering, University of Chicago（芝加哥大学普里茨克分子工程学院）；Department of Chemistry, James Franck Institute, University of Chicago（芝加哥大学化学系、詹姆斯·弗兰克研究所）；Department of Materials Science and Engineering, Rensselaer Polytechnic Institute（伦斯勒理工学院材料科学与工程系）；X-ray Science Division, Advanced Photon Source, Argonne National Laboratory（阿贡国家实验室先进光子源部X射线科学分部）；Center for Nanoscale Materials, Argonne National Laboratory（阿贡国家实验室纳米材料中心）；Electron Microscopy Core, University of Illinois Chicago（伊利诺伊大学芝加哥分校电子显微镜核心设施）
Hole-doped perovskite bismuthates such as Ba$_{1-x}$K$_x$BiO$_3$ and Sr$_{1-x}$K$_x$BiO$_3$ are well-known bismuth-based oxide high-transition-temperature superconductors. Reported thin bismuthate films show relatively low quality, likely due to their large lattice mismatch with the substrate and a low sticking coefficient of Bi at high temperatures. Here, we report the successful epitaxial thin film growth of the parent compound strontium bismuthate SrBiO$_3$ on SrO-terminated SrTiO$_3$ (001) substrates by molecular beam epitaxy. Two different growth methods, high-temperature co-deposition or…
Molecular beam epitaxy offers an exciting avenue for investigating the behavior of topological semimetal Cd3As2, by providing routes for doping, alloying, strain engineering, and heterostructure formation. To date, however, minimal exploration has been devoted to the impact of defects that are incorporated into epilayers due to contraints imposed by the substrate and narrow growth window. Here, we use a combination of lattice-matched ZnxCd1-xTe buffer layers, miscut substrates and broadband illumination to study how dislocations, twins and point defects influence the electron mobility of Cd3As…
We demonstrate a novel route to prepare thin films of the ferromagnetic insulator Europium monoxide. Key is a redox-controlled interface reaction between metallic Eu and the substrate SrTiO$_3$ as the supplier of oxygen. The process allows tuning the electronic, magnetic and structural properties of the EuO films. Furthermore, we apply this technique to various oxidic substrates and demonstrate the universality and limits of a redox-controlled EuO film synthesis.
Epitaxy of ZnO layers on cubic GaP (111) substrates has been demonstrated using pulsed laser deposition. Out of plane and in-plane epitaxial relationship of ZnO layer with respect to GaP substrate determined using phi scans in high resolution X-ray diffraction measurements are (0001) ZnO || (111) GaP and (-1 2 -1 0) ZnO || (-1 1 0) GaP respectively. Our results of epitaxy of ZnO and its intense excitonic photoluminescence with very weak defect luminescence suggest that (111) oriented GaP can be a potential buffer layer choice for the integration of ZnO based optoelectronic devices on Si(111) s…
Epitaxy of oxide materials on silicon (Si) substrates is of great interest for future functional devices using the large variety of physical properties of the oxides as ferroelectricity, ferromagnetism, or superconductivity. Recently, materials with high spin polarization of the charge carriers have become interesting for semiconductor-oxide hybrid devices in spin electronics. Here, we report on pulsed laser deposition of magnetite (Fe3O4) on Si(001) substrates cleaned by an in situ laser beam high temperature treatment. After depositing a double buffer layer of titanium nitride (TiN) and magn…
Smooth interfaces and surfaces are beneficial for most (opto)electronic devices based on thin films and their heterostructures. For example, smoother interfaces in (010) beta-Ga2O3/(AlxGa1-x)2O3 heterostructures, whose roughness is ruled by that of the Ga2O3 layer, can enable higher mobility 2DEGs by reducing interface roughness scattering. To this end we experimentally prove that a substrate offcut along the [001] direction allows to obtain smooth beta-Ga2O3 layers in (010)-homoepitaxy under metal-rich conditions. Applying In-mediated metal-exchange catalysis (MEXCAT) in molecular beam epitax…
Images of uniform and upright nanowires are fascinating, but often, they are quite puzzling, when epitaxial templating from the substrate is clearly absent. Here, we reveal the physics underlying one such hidden growth guidance mechanism through a specific example - the case of ZnO nanowires grown on silicon oxide and glass. We show how electric fields exerted by the insulating substrate may be manipulated through the surface charge to define the orientation and polarity of the nanowires. Surface charge is ubiquitous on the surfaces of semiconductors and insulators, and as a result, substrate …
Topological quantum computing is based on braiding of Majorana zero modes encoding topological qubits. A promising candidate platform for Majorana zero modes is semiconductor-superconductor hybrid nanowires. The realization of topological qubits and braiding operations requires scalable and disorder-free nanowire networks. Selective area growth of in-plane InAs and InSb nanowires, together with shadow-wall growth of superconductor structures, have demonstrated this scalability by achieving various network structures. However, the noticeable lattice mismatch at the nanowire-substrate interface,…
Superconducting thin films of magnesium diboride (MgB$_2$) were prepared on MgO (001) substrate by a molecular beam epitaxy (MBE) method with the co-evaporation conditions of low deposition rate in ultra-high vacuum. The structural and physical properties of the films were studied by RHEED, XRD, XPS, resistivity and magnetization measurements.All films demonstrated superconductivity without use of any post-annealing process.The highest {\it T}$_{c,onset}$ determined by resistivity measurement was about 33K in the present samples.Anisotropic superconducting properties were evaluated by the resi…
In this work we investigate the growth of $β$-Ga2O3 homoepitaxial layers on top of (100) oriented substrates via indium-assisted metal exchange catalyzed molecular beam epitaxy (MEXCAT-MBE) which have exhibited prohibitively low growth rates by non-catalyzed MBE in the past. We demonstrate that the proper tuning of the MEXCAT growth parameters and the choice of a proper substrate offcut allow for the deposition of thin films with high structural quality via step-flow growth mechanism at relatively high growth rates for $β$-Ga2O3 homoepitaxy (i.e., around 1.5 nm/min, $\approx$45% incorporation …
