The growth of graphene by catalytic decomposition of ethylene on Cu(111) in an ultra-high vacuum system was investigated with low energy electron diffraction, low energy electron microscopy, and atomic force microscopy. Attempts to form a graphene overlayer using ethylene at pressures as high as 10 mTorr and substrate temperatures as high as 900 • C resulted in almost no graphene growth. By using an argon overpressure, the growth of epitaxial graphene on Cu(111) was achieved.The suppression of graphene growth without the use of an argon overpressure is attributed to Cu sublimation at elevated temperatures. During the initial stages of growth, a random distribution of rounded graphene islands is observed. The predominant rotational orientation of the islands is within ±1 • of the Cu(111) substrate lattice.
The topologically protected surface states of three-dimensional (3D) topological insulators have the potential to be transformative for high-performance logic and memory devices by exploiting their specific properties such as spin-polarized current transport and defect tolerance due to suppressed backscattering. However, topological insulator based devices have been underwhelming to date primarily due to the presence of parasitic issues. An important example is the challenge of suppressing bulk conduction in BiSe and achieving Fermi levels ( E) that reside in between the bulk valence and conduction bands so that the topologically protected surface states dominate the transport. The overwhelming majority of the BiSe studies in the literature report strongly n-type materials with E in the bulk conduction band due to the presence of a high concentration of selenium vacancies. In contrast, here we report the growth of near-intrinsic BiSe with a minimal Se vacancy concentration providing a Fermi level near midgap with no extrinsic counter-doping required. We also demonstrate the crucial ability to tune E from below midgap into the upper half of the gap near the conduction band edge by controlling the Se vacancy concentration using post-growth anneals. Additionally, we demonstrate the ability to maintain this Fermi level control following the careful, low-temperature removal of a protective Se cap, which allows samples to be transported in air for device fabrication. Thus, we provide detailed guidance for E control that will finally enable researchers to fabricate high-performance devices that take advantage of transport through the topologically protected surface states of BiSe.
Understanding the influence that copper substrate surface symmetry and oxygen impurities have on the growth of graphene by chemical vapor deposition is important for developing techniques for producing high quality graphene. Therefore, we have studied the growth of graphene by catalytic decomposition of ethylene in an ultra-high vacuum chamber on both a clean Cu(100) surface and a Cu(100) surface pre-dosed with a layer of chemisorbed oxygen.The crystal structure of the graphene films was characterized with in-situ low energy electron diffraction. By heating the clean Cu(100) substrate from room temperature to the growth temperature in ethylene, epitaxial graphene films were formed. The crystal quality was found to depend strongly on the growth temperature. At 900 • C, well-ordered two-domain graphene films were formed. Pre-dosing the Cu(100) surface with a chemisorbed layer of oxygen before graphene growth was found to adversely affect the crystal quality of the graphene overlayer by inducing a much higher degree of rotational disorder of the graphene grains with respect to the Cu(100) substrate. The growth morphology of the graphene islands during the initial stages of nucleation was monitored with ex-situ scanning electron microscopy. The nucleation rate of the graphene islands was observed to drop by an order of magnitude by pre-dosing the Cu (100) surface with a chemisorbed oxygen layer before growth. This reduction in nucleation rate results in the formation of much larger graphene islands. Therefore, the presence of oxygen during graphene growth affects both the relative orientation and average size of grains within the films grown on Cu(100) substrates.
Intelligent engineering of graphene-based electronic devices on SiC(0001) requires a better understanding of processes used to deposit gate-dielectric materials on graphene. Recently, Al2O3 dielectrics have been shown to form conformal, pinhole-free thin films by functionalizing the top surface of the graphene with fluorine prior to atomic layer deposition (ALD) of the Al2O3 using a trimethylaluminum (TMA) precursor. In this work, the functionalization and ALD-precursor adsorption processes have been studied with angle-resolved photoelectron spectroscopy, low energy electron diffraction, and X-ray photoelectron spectroscopy. It has been found that the functionalization process has a negligible effect on the electronic structure of the graphene, and that it results in a twofold increase in the adsorption of the ALD-precursor. In situ TMA-dosing and XPS studies were also performed on three different Si(100) substrates that were terminated with H, OH, or dangling Si-bonds. This dosing experiment revealed that OH is required for TMA adsorption. Based on those data along with supportive in situ measurements that showed F-functionalization increases the amount of oxygen (in the form of adsorbed H2O) on the surface of the graphene, a model for TMA-adsorption on graphene is proposed that is based on a reaction of a TMA molecule with OH.
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