Interests in two-dimensional transition-metal dichalcogenides have prompted some recent efforts to grow ultrathin layers of these materials epitaxially using molecular-beam epitaxy. However, growths of monolayer and bilayer WSe2, an important member of the transition-metal dichalcogenides family, by the molecular-beam epitaxy method remain uncharted probably because of the difficulty in generating tungsten fluxes from the elemental source. In this work, we present a scanning tunneling microscopy and spectroscopy study of molecular-beam epitaxy-grown WSe2 monolayer and bilayer, showing atomically flat epifilm with no domain boundary defect. This contrasts epitaxial MoSe2 films grown by the same method, where a dense network of the domain boudaries defects is present. The scanning tunneling spectroscopy measurements of monolayer and bilayer WSe2 domains of the same sample reveal not only the bandgap narrowing upon increasing the film thickness from monolayer to bilayer, but also a band-bending effect across the boundary between monolayer and bilayer domains. This band-bending appears to be dictated by the edge states at steps of the bilayer islands. Finally, comparison is made between the scanning tunneling spectroscopy-measured electronic bandgaps with the exciton emission energies measured by photoluminescence, and the exciton binding energies in monolayer and bilayer WSe2/MoSe2 are thus estimated.
We present a combined experimental and theoretical study of monolayer VTe2 grown on highly oriented pyrolytic graphite by molecular-beam epitaxy. Using various in-situ microscopic and spectroscopic techniques, including scanning tunneling microscopy/spectroscopy, synchrotron X-ray and angle-resolved photoemission, and X-ray absorption, together with theoretical analysis by density functional theory calculations, we demonstrate direct evidence of the metallic 1T phase and 3d1 electronic configuration in monolayer VTe2 that also features a (4 x 4) charge density wave order at low temperatures. I…
The structure of the ultimately-thin crystalline allotrope of silicon oxide, prepared onto a ruthenium surface, is unveiled down to atomic scale with chemical sensitivity, thanks to high resolution scanning tunneling microscopy and first principle calculations. An ordered oxygen lattice is imaged which coexists with the two-dimensional monolayer oxide. This coexistence signals a displacive transformation from an oxygen reconstructed-Ru(0001) to silicon oxide, along which latterally-shifted domains form, each with equivalent and degenerate epitaxial relationships with the substrate. The unavoid…
$WSe_2$ Monolayers Grown by Molecular Beam Epitaxy on hBN
Institute of Experimental Physics, Faculty of Physics, University of Warsaw（华沙大学物理学院实验物理研究所）；Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（国家材料科学研究所材料纳米构造研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（国家材料科学研究所电子与光学材料研究中心）
Monolayer (ML) transition-metal dichalcogenides exist in different phases, such as the hexagonal (2H) and distorted octahedral or monoclinic (1T') phases. The different structures show vastly different properties. For example, the 2H MoTe2 ML is a direct-gap semiconductor while 1T' MoTe2 is a semi-metal. It has been suggested that the formation energies between 2H and 1T' MoTe2 differ very little, so there is a high chance to tune the structures of MoTe2 and thereby to bring in new applications such as phase-change electronics. In this work, we report growth of both 2H and 1T' MoTe2 ML by mole…
We have performed Kinetic Monte Carlo simulation to study the effect of diffusion anisotropy and bonding anisotropy 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 Kinetic Monte Carlo method to simulate the physical phenomena. We have found that surface anisotropy has no significant role on island elongation however it influences on the island morphology, growth exponent and island size distribution. Elongated islands were obtained…
The search for high-quality transition metal dichalcogenides mono- and multi-layers grown on large areas is still a very active field of investigation nowadays. Here, we use molecular beam epitaxy to grow 15$\times$15 mm large WSe$_2$ on mica in the van der Waals regime. By screening one-step growth conditions, we find that very high temperature ($>$900$^{\circ}$C) and very low deposition rate ($<$0.015 nm/min) are necessary to obtain high quality WSe$_2$ films. The domain size can be larger than 1 $μ$m and the in-plane rotational misorientation less than $\pm$0.5$^{\circ}$. The WSe$_2$ monola…
Research on two-dimensional materials has expanded over the past two decades to become a central theme in condensed matter research today. Significant advances have been made in the synthesis and subsequent reassembly of these materials using mechanical methods into a vast array of hybrid structures with novel properties and ever-increasing potential applications. The key hurdles in realizing this potential are the challenges in controlling the atomic structure of these layered hybrid materials and the difficulties in harnessing their unique functionality with existing semiconductor nanofabric…
Two-dimensional materials (2D) arranged in hybrid van der Waals (vdW) heterostructures provide a route toward the assembly of 2D and conventional III-V semiconductors. Here, we report the structural and electronic properties of single layer WSe2 grown by molecular beam epitaxy on Se-terminated GaAs(111)B. Reflection high-energy electron diffraction images exhibit sharp streaky features indicative of a high-quality WSe2 layer produced via vdW epitaxy. This is confirmed by in-plane x-ray diffraction. The single layer of WSe2 and the absence of interdiffusion at the interface are confirmed by hig…
Interfacial Coupling Controls Molecular Epitaxy of HMTP on Graphene/SiC
Masaryk University（马萨里克大学）；Brno University of Technology（布尔诺理工大学）；Charles University（查理大学）；Institute of Physical Engineering, Brno University of Technology（布尔诺理工大学物理工程学院）
Epitaxy forms the basis of modern electronics and optoelectronics. We report coherent atomically-thin superlattices, in which different transition metal dichalcogenide monolayers--despite large lattice mismatches--are repeated and integrated without dislocations. Grown by a novel omnidirectional epitaxy, these superlattices display fully-matched lattice constants across heterointerfaces while maintaining a surprisingly isotropic lattice structure and triangular symmetry. This strong epitaxial strain is precisely engineered via the nanoscale supercell dimensions, thereby enabling broad tuning o…
Two-dimensional (2D) semiconductor of MoS2 has great potential for advanced electronics technologies beyond silicon1-9. So far, high-quality monolayer MoS2 wafers10-12 are already available and various demonstrations from individual transistors to integrated circuits have also been shown13-15. In addition to the monolayer, multilayers have narrower band gaps but improved carrier mobilities and current capacities over the monolayer5,16-18. However, achieving high-quality multilayer MoS2 wafers remains a challenge. Here we report the growth of high quality multilayer MoS2 4-inch wafers via the l…
Epitaxial growth of atomically-sharp interfaces serves as one of the main building blocks of nanofabrication. Such interfaces are crucial for the operation of various devices including transistors, photo-voltaic cells, and memory components. In order to avoid charge traps that may hamper the operation of such devices, it is critical for the layers to be atomically-sharp. Fabrication of atomically sharp interfaces normally requires ultra-high vacuum techniques and high substrate temperatures. We present here a new self-limiting wet chemical process for deposition of epitaxial layers from alkoxi…
We report epitaxial growth of vanadium diselenide (VSe$_2$) thin films in the octahedrally-coordinated (1T) structure on GaAs(111)B substrates by molecular beam epitaxy. Film thickness from a single monolayer (ML) up to 30 ML is demonstrated. Structural and chemical studies using by x-ray diffraction, transmission electron microscopy, scanning tunneling microscopy and x-ray photoelectron spectroscopy indicate high quality thin films. Further studies show that monolayer VSe$_2$ films on GaAs are not air-stable and are susceptible to oxidation within a matter of hours, which indicates that a pro…
Realizing van der Waals (vdW) epitaxy in the 80s represents a breakthrough that circumvents the stringent lattice matching and processing compatibility requirements in conventional covalent heteroepitaxy. However, due to the weak vdW interactions, there is little control over film qualities by the substrate. Typically, discrete domains with a spread of misorientation angles are formed, limiting the applicability of vdW epitaxy. Here we report the epitaxial growth of monocrystalline, covalent Cr5Te8 2D crystals on monolayer vdW WSe2 by chemical vapor deposition, driven by interfacial dative bon…
Monolayer Tellurium (Te) or tellurene has been suggested by a recent theory as a new two-dimensional (2D) system with great electronic and optoelectronic promises. Here we present an experimental study of epitaxial Te deposited on highly oriented pyrolytic graphite (HOPG) substrate by molecular-beam epitaxy. Scanning tunneling microscopy of ultrathin layers of Te reveals rectangular surface cells with the cell size consistent with the theoretically predicted beta-tellurene, whereas for thicker films, the cell size is more consistent with that of the (10-10) surface of bulk Te crystal. Scanning…
PtSe2 is attracting considerable attention as a high mobility two-dimensional material with envisionned applications in microelectronics, photodetection and spintronics. The growth of high quality PtSe2 on insulating substrates with wafer-scale uniformity is a prerequisite for electronic transport investigations and practical use in devices. Here, we report the growth of highly oriented few-layers PtSe2 on ZnO(0001) by molecular beam epitaxy. The crystalline structure of the films is characterized with electron and X-ray diffraction, atomic force microscopy and transmission electron microscopy…
Using four-wave mixing microscopy, we measure the coherent response and ultrafast dynamics of excitons and trions in MoSe$_2$ monolayers grown by molecular beam epitaxy on thin films of hexagonal boron nitride. We assess inhomogeneous and homogeneous broadenings in the transition spectral lineshape. The impact of phonons on the homogeneous dephasing is inferred via the temperature dependence of the dephasing. Four-wave mixing mapping, combined with the atomic force microscopy, reveals spatial correlations between exciton oscillator strength, inhomogeneous broadening and the sample morphology. …
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 report the structural and optical properties of molecular beam epitaxy (MBE) grown 2-dimensional (2D) material molybdenum diselenide (MoSe2) on graphite, CaF2 and epitaxial graphene. Extensive characterizations reveal that 2H- MoSe2 grows by van-der-Waals epitaxy on all 3 substrates with a preferred crystallographic orientation and a Mo:Se ratio of 1:2. Photoluminescence at room temperature (~1.56 eV) is observed in monolayer MoSe2 on both CaF2 and epitaxial graphene. The band edge absorption is very sharp, <60 meV over 3 decades. Overcoming the observed small grains by promoting mobility o…
Two-dimensional lateral heterojunctions are basic components for low-power and flexible optoelectronics. In contrast to monolayers, devices based on few-layer lateral heterostructures could offer superior performance due to their lower susceptibility to environmental conditions. Here, we report the controlled synthesis of multi-junction bilayer lateral heterostructures based on MoS2-WS2 and MoSe2-WSe2, where the hetero-junctions are created via sequential lateral edge-epitaxy that happens simultaneously in both the first and the second layer. With respect to their monolayer counterparts, bilay…
Very recently, it was demonstrated that the carrier mobility of a molecular monolayer dioctylbenzothienobenzothiophene (C8-BTBT) on boron nitride can reach 10 cm2/Vs, the highest among the previously reported monolayer molecular field-effect transistors. Here we show that the high-quality single crystal of the C8-BTBT monolayer may be the key origin of the record-high carrier mobility. We discover that the C8-BTBT molecules prefer layer-by-layer growth on both hexagonal boron nitride and graphene. The flatness of these substrates substantially decreases the C8-BTBT nucleation density and enabl…
Mirror twin boundary (MTB) brings unique 1D physics and properties into two-dimensional transition metal dichalcogenides (TMDCs), but they were rarely observed in non-Mo-based TMDCs. Herein, by post-growth Nb doping, high density 4|4E-W and 4|4P-Se MTBs were introduced into molecular beam epitaxy (MBE) grown WSe2 monolayers. Of them, 4|4E-W MTB with a novel structure was discovered experimentally for the first time, while 4|4P-Se MTBs present a random permutations of W and Nb, forming a 1D alloy system. Comparison between the doped and non-doped WSe2 confirmed that Nb dopants are essential for…
The strong light-matter interaction in transition Metal dichalcogenides (TMDs) monolayers (MLs) is governed by robust excitons. Important progress has been made to control the dielectric environment surrounding the MLs, especially through hexagonal boron nitride (hBN) encapsulation, which drastically reduces the inhomogeneous contribution to the exciton linewidth. Most studies use exfoliated hBN from high quality flakes grown under high pressure. In this work, we show that hBN grown by molecular beam epitaxy (MBE) over a large surface area substrate has a similarly positive impact on the optic…
Molecular beam epitaxy of wafer-scale O-band InAs/InGaAs quantum dots on GaAs for quantum photonics
Technical University of Munich（慕尼黑工业大学）；TUM School of Computation, Information and Technology, Technical University of Munich（慕尼黑工业大学计算、信息与技术学院）；Julius-Maximilians-Universität Würzburg（维尔茨堡大学）；Saqura Technologies GmbH（萨库拉技术有限公司）；Ruhr University Bochum（波鸿鲁尔大学）；Ludwig-Maximilians-University Munich（慕尼黑大学）；Technical University Berlin（柏林工业大学）；Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院）
High quality WSe2 films have been grown on bilayer graphene (BLG) with layer-by-layer control of thickness using molecular beam epitaxy (MBE). The combination of angle-resolved photoemission (ARPES), scanning tunneling microscopy/spectroscopy (STM/STS), and optical absorption measurements reveal the atomic and electronic structures evolution and optical response of WSe2/BLG. We observe that a bilayer of WSe2 is a direct bandgap semiconductor, when integrated in a BLG-based heterostructure, thus shifting the direct-indirect band gap crossover to trilayer WSe2. In the monolayer limit, WSe2 shows…
Chemical vapor deposition (CVD) allows lateral edge epitaxy of transition metal dichalcogenide heterostructures with potential applications in optoelectronics. Critical for carrier and exciton transport is the quality of the two materials that constitute the monolayer and the nature of the lateral heterojunction. Important details of the optical properties were inaccessible in as-grown heterostructure samples due to large inhomogeneous broadening of the optical transitions. Here we perform optical spectroscopy at T = 4 K and also at 300 K to access the optical transitions in CVD grown MoSe2-WS…
The stacked two layered materials with a lattice constant mismatch and/or with twist angle relative to each other can create a moiré pattern, modulating the electronic properties of the pristine materials. Here, we combine scanning tunneling microscopy/spectroscopy and density functional theory calculations to investigate the moiré potential induced bandgap tuning in InSe/CuSe vertical heterostructure synthesized by a two-step of molecular beam epitaxy. Scanning tunneling microscopy measurements demonstrate the heterostructure with a superlattice periodicity of ~3.48nm and a twist angle of abo…
Bilayer (BL) MoSe2 films grown by molecular-beam epitaxy (MBE) are studied by scanning tunneling microscopy and spectroscopy (STM/S). Similar to monolayer (ML) films, networks of inversion domain boundary (DB) defects are observed both in the top and bottom layers of BL MoSe2, and often they are seen spatially correlated such that one is on top of the other. There are also isolated ones in the bottom layer without companion in the top-layer and are detected by STM/S through quantum tunneling of the defect states through the barrier of the MoSe2 ML. Comparing the DB states in BL MoSe2 with that…
Two-dimensional van der Waals crystals arise limitless scope for designing novel combinations of physical properties via controlling the stacking order or twist angle of individual layers. Lattice orientation between stacked monolayers is significant not only for the engineering symmetry breaking but also for the study of many-body quantum phases and band topology. So far the state-of-art exfoliation approaches focusing on achievements of quality, size, yield, and scalability while lacking sufficient information on lattice orientation. Consequently, interlayer alignment is usually determined b…
