High-Quality Few-Layer Graphene on Single-Crystalline SiC thin Film Grown on Affordable Wafer for Device Applications.

Graphene is promising for next-generation devices. However, one of the primary challenges in realizing these devices is the scalable growth of high-quality few-layer graphene (FLG) on device-type wafers; it is difficult to do so while balancing both quality and affordability. High-quality graphene is grown on expensive SiC bulk crystals, while graphene on SiC thin films grown on Si substrates (GOS) exhibits low quality but affordable cost. We propose a new method for the growth of high-quality FLG on a new template named "hybrid SiC". The hybrid SiC is produced by bonding a SiC bulk crystal with an affordable device-type wafer and subsequently peeling off the SiC bulk crystal to obtain a single-crystalline SiC thin film on the wafer. The quality of FLG on this hybrid SiC is comparable to that of FLG on SiC bulk crystals and much higher than of GOS. FLG on the hybrid SiC exhibited high carrier mobilities, comparable to those on SiC bulk crystals, as anticipated from the linear band dispersions. Transistors using FLG on the hybrid SiC showed the potential to operate in terahertz frequencies. The proposed method is suited for growing high-quality FLG on desired substrates with the aim of realizing graphene-based high-speed devices.

Ultrafast Unbalanced Electron Distributions in Quasicrystalline 30° Twisted Bilayer Graphene.

Ultrafast carrier dynamics in a graphene system are very important in terms of optoelectronic devices. Recently, a twisted bilayer graphene has been discovered that possesses interesting electronic properties owing to strong modifications in interlayer couplings. Thus, a better understanding of ultrafast carrier dynamics in a twisted bilayer graphene is highly desired. Here, we reveal the unbalanced electron distributions in a quasicrystalline 30° twisted bilayer graphene (QCTBG), using time- and angle-resolved photoemission spectroscopy on the femtosecond time scale. We distinguish time-dependent electronic behavior between the upper- and lower-layer Dirac cones and gain insight into the dynamical properties of replica bands, which show characteristic signatures due to Umklapp scatterings. The experimental results are reproduced by solving a set of rate equations among the graphene layers and substrate. We find that the substrate buffer layer plays a key role in initial carrier injections to the upper and lower layers. Our results demonstrate that QCTBG can be a promising element for future devices.

Operation Mechanism of GaN-based Transistors Elucidated by Element-Specific X-ray Nanospectroscopy.

With the rapid depletion of communication-frequency resources, mainly due to the explosive spread of information communication devices for the internet of things, GaN-based high-frequency high-power transistors (GaN-HEMTs) have attracted considerable interest as one of the key devices that can operate in the high-frequency millimeter-wave band. However, GaN-HEMT operation is destabilized by current collapse phenomena arising from surface electron trapping (SET), which has not been fully understood thus far. Here, we conduct quantitative mechanistic studies on SET in GaN-HEMTs by applying element- and site-specific photoelectron nanospectroscopy to a GaN-HEMT device under operation. Our study reveals that SET is induced by a large local electric field. Furthermore, surface passivation using a SiN thin film is demonstrated to play a dual role: electric-field weakening and giving rise to chemical interactions that suppress SET. Our findings can contribute to the realization of high-capacity wireless communication systems based on GaN-HEMTs.

Enhancement of CO2 adsorption on oxygen-functionalized epitaxial graphene surface under near-ambient conditions.

The functionalization of graphene is important in practical applications of graphene, such as in catalysts. However, the experimental study of the interactions of adsorbed molecules with functionalized graphene is difficult under ambient conditions at which catalysts are operated. Here, the adsorption of CO2 on an oxygen-functionalized epitaxial graphene surface was studied under near-ambient conditions using ambient-pressure X-ray photoelectron spectroscopy (AP-XPS). The oxygen-functionalization of graphene is achieved in situ by the photo-induced dissociation of CO2 with X-rays on graphene in a CO2 gas atmosphere. The oxygen species on the graphene surface is identified as the epoxy group by XPS binding energies and thermal stability. Under near-ambient conditions of 1.6 mbar CO2 gas pressure and 175 K sample temperature, CO2 molecules are not adsorbed on the pristine graphene, but are adsorbed on the oxygen-functionalized graphene surface. The increase in the adsorption energy of CO2 on the oxygen-functionalized graphene surface is supported by first-principles calculations with the van der Waals density functional (vdW-DF) method. The adsorption of CO2 on the oxygen-functionalized graphene surface is enhanced by both the electrostatic interactions between the CO2 and the epoxy group and the vdW interactions between the CO2 and graphene. The detailed understanding of the interaction between CO2 and the oxygen-functionalized graphene surface obtained in this study may assist in developing guidelines for designing novel graphene-based catalysts.

In Situ SR-XPS Observation of Ni-Assisted Low-Temperature Formation of Epitaxial Graphene on 3C-SiC/Si.

Low-temperature (~1073 K) formation of graphene was performed on Si substrates by using an ultrathin (2 nm) Ni layer deposited on a 3C-SiC thin film heteroepitaxially grown on a Si substrate. Angle-resolved, synchrotron-radiation X-ray photoemission spectroscopy (SR-XPS) results show that the stacking order is, from the surface to the bulk, Ni carbides(Ni3C/NiCx)/graphene/Ni/Ni silicides (Ni2Si/NiSi)/3C-SiC/Si. In situ SR-XPS during the graphitization annealing clarified that graphene is formed during the cooling stage. We conclude that Ni silicide and Ni carbide formation play an essential role in the formation of graphene.

Interfacial Charge States in Graphene on SiC Studied by Noncontact Scanning Nonlinear Dielectric Potentiometry.

We investigate pristine and hydrogen-intercalated graphene synthesized on a 4H-SiC(0001) substrate by using noncontact scanning nonlinear dielectric potentiometry (NC-SNDP). Permanent dipole moments are detected at the pristine graphene-SiC interface. These originate from the covalent bonds of carbon atoms of the so-called buffer layer to the substrate. Hydrogen intercalation at the interface eliminates these covalent bonds and the original quasi-(6×6) corrugation, which indicates the conversion of the buffer layer into a second graphene layer by the termination of Si bonds at the interface. NC-SNDP images suggest that a certain portion of the Si dangling bonds remains even after hydrogen intercalation. These bonds are thought to act as charged impurities reducing the carrier mobility in hydrogen-intercalated graphene on SiC.

Microscopically-tuned band structure of epitaxial graphene through interface and stacking variations using Si substrate microfabrication.

Graphene exhibits unusual electronic properties, caused by a linear band structure near the Dirac point. This band structure is determined by the stacking sequence in graphene multilayers. Here we present a novel method of microscopically controlling the band structure. This is achieved by epitaxy of graphene on 3C-SiC(111) and 3C-SiC(100) thin films grown on a 3D microfabricated Si(100) substrate (3D-GOS (graphene on silicon)) by anisotropic etching, which produces Si(111) microfacets as well as major Si(100) microterraces. We show that tuning of the interface between the graphene and the 3C-SiC microfacets enables microscopic control of stacking and ultimately of the band structure of 3D-GOS, which is typified by the selective emergence of semiconducting and metallic behaviours on the (111) and (100) portions, respectively. The use of 3D-GOS is thus effective in microscopically unlocking various potentials of graphene depending on the application target, such as electronic or photonic devices.

Orbital-specific tunability of many-body effects in bilayer graphene by gate bias and metal contact.

Graphene, a 2D crystal bonded by π and σ orbitals, possesses excellent electronic properties that are promising for next-generation optoelectronic device applications. For these a precise understanding of quasiparticle behaviour near the Dirac point (DP) is indispensable because the vanishing density of states (DOS) near the DP enhances many-body effects, such as excitonic effects and the Anderson orthogonality catastrophe (AOC) which occur through the interactions of many conduction electrons with holes. These effects renormalize band dispersion and DOS, and therefore affect device performance. For this reason, we have studied the impact of the excitonic effects and the AOC on graphene device performance by using X-ray absorption spectromicroscopy on an actual graphene transistor in operation. Our work shows that the excitonic effect and the AOC are tunable by gate bias or metal contacts, both of which alter the Fermi energy, and are orbital-specific.

Surface Chemistry Involved in Epitaxy of Graphene on 3C-SiC(111)/Si(111).

Surface chemistry involved in the epitaxy of graphene by sublimating Si atoms from the surface of epitaxial 3C-SiC(111) thin films on Si(111) has been studied. The change in the surface composition during graphene epitaxy is monitored by in situ temperature-programmed desorption spectroscopy using deuterium as a probe (D(2)-TPD) and complementarily by ex situ Raman and C1s core-level spectroscopies. The surface of the 3C-SiC(111)/Si(111) is Si-terminated before the graphitization, and it becomes C-terminated via the formation of C-rich (6√3 × 6√3)R30° reconstruction as the graphitization proceeds, in a similar manner as the epitaxy of graphene on Si-terminated 6H-SiC(0001) proceeds.