Haomin Wang

Fast growth of inch-sized single-crystalline graphene from a controlled single nucleus on Cu–Ni alloys

Wafer-scale single-crystalline graphene monolayers are highly sought after as an ideal platform for electronic and other applications. At present, state-of-the-art growth methods based on chemical vapour deposition allow the synthesis of one-centimetre-sized single-crystalline graphene domains in ∼12 h, by suppressing nucleation events on the growth substrate. Here we demonstrate an efficient strategy for achieving large-area single-crystalline graphene by letting a single nucleus evolve into a monolayer at a fast rate. By locally feeding carbon precursors to a desired position of a substrate composed of an optimized Cu-Ni alloy, we synthesized an ∼1.5-inch-large graphene monolayer in 2.5 h. Localized feeding induces the formation of a single nucleus on the entire substrate, and the optimized alloy activates an isothermal segregation mechanism that greatly expedites the growth rate. This approach may also prove effective for the synthesis of wafer-scale single-crystalline monolayers of other two-dimensional materials.

Synthesis of large single-crystal hexagonal boron nitride grains on Cu–Ni alloy

Hexagonal boron nitride (h-BN) has attracted significant attention because of its superior properties as well as its potential as an ideal dielectric layer for graphene-based devices. The h-BN films obtained via chemical vapour deposition in earlier reports are always polycrystalline with small grains because of high nucleation density on substrates. Here we report the successful synthesis of large single-crystal h-BN grains on rational designed Cu-Ni alloy foils. It is found that the nucleation density can be greatly reduced to 60 per mm(2) by optimizing Ni ratio in substrates. The strategy enables the growth of single-crystal h-BN grains up to 7,500 μm(2), approximately two orders larger than that in previous reports. This work not only provides valuable information for understanding h-BN nucleation and growth mechanisms, but also gives an effective alternative to exfoliated h-BN as a high-quality dielectric layer for large-scale nanoelectronic applications.

Precisely aligned graphene grown on hexagonal boron nitride by catalyst free chemical vapor deposition.

To grow precisely aligned graphene on h-BN without metal catalyst is extremely important, which allows for intriguing physical properties and devices of graphene/h-BN hetero-structure to be studied in a controllable manner. In this report, such hetero-structures were fabricated and investigated by atomic resolution scanning probe microscopy. Moiré patterns are observed and the sensitivity of moiré interferometry proves that the graphene grains can align precisely with the underlying h-BN lattice within an error of less than 0.05°. The occurrence of moiré pattern clearly indicates that the graphene locks into h-BN via van der Waals epitaxy with its interfacial stress greatly released. It is worthy to note that the edges of the graphene grains are primarily oriented along the armchair direction. The field effect mobility in such graphene flakes exceeds 20,000 cm2·V−1·s−1 at ambient condition. This work opens the door of atomic engineering of graphene on h-BN, and sheds light on fundamental research as well as electronic applications based on graphene/h-BN hetero-structure.

Silane-catalysed fast growth of large single-crystalline graphene on hexagonal boron nitride

The direct growth of high-quality, large single-crystalline domains of graphene on a dielectric substrate is of vital importance for applications in electronics and optoelectronics. Traditionally, graphene domains grown on dielectrics are typically only ~1 μm with a growth rate of ~1 nm min−1 or less, the main reason is the lack of a catalyst. Here we show that silane, serving as a gaseous catalyst, is able to boost the graphene growth rate to ~1 μm min−1, thereby promoting graphene domains up to 20 μm in size to be synthesized via chemical vapour deposition (CVD) on hexagonal boron nitride (h-BN). Hall measurements show that the mobility of the sample reaches 20,000 cm2 V−1 s−1 at room temperature, which is among the best for CVD-grown graphene. Combining the advantages of both catalytic CVD and the ultra-flat dielectric substrate, gaseous catalyst-assisted CVD paves the way for synthesizing high-quality graphene for device applications while avoiding the transfer process.

Oriented graphene nanoribbons embedded in hexagonal boron nitride trenches

Graphene nanoribbons (GNRs) are ultra-narrow strips of graphene that have the potential to be used in high-performance graphene-based semiconductor electronics. However, controlled growth of GNRs on dielectric substrates remains a challenge. Here, we report the successful growth of GNRs directly on hexagonal boron nitride substrates with smooth edges and controllable widths using chemical vapour deposition. The approach is based on a type of template growth that allows for the in-plane epitaxy of mono-layered GNRs in nano-trenches on hexagonal boron nitride with edges following a zigzag direction. The embedded GNR channels show excellent electronic properties, even at room temperature. Such in-plane hetero-integration of GNRs, which is compatible with integrated circuit processing, creates a gapped channel with a width of a few benzene rings, enabling the development of digital integrated circuitry based on GNRs.

High- T c superconductivity in ultrathin Bi 2 Sr 2 CaCu 2 O 8+ x down to half-unit-cell thickness by protection with graphene

High-Tc superconductors confined to two dimension exhibit novel physical phenomena, such as superconductor-insulator transition. In the Bi2Sr2CaCu2O(8+x) (Bi2212) model system, despite extensive studies, the intrinsic superconducting properties at the thinness limit have been difficult to determine. Here, we report a method to fabricate high quality single-crystal Bi2212 films down to half-unit-cell thickness in the form of graphene/Bi2212 van der Waals heterostructure, in which sharp superconducting transitions are observed. The heterostructure also exhibits a nonlinear current-voltage characteristic due to the Dirac nature of the graphene band structure. More interestingly, although the critical temperature remains essentially the same with reduced thickness of Bi2212, the slope of the normal state T-linear resistivity varies by a factor of 4-5, and the sheet resistance increases by three orders of magnitude, indicating a surprising decoupling of the normal state resistance and superconductivity. The developed technique is versatile, applicable to investigate other two-dimensional (2D) superconducting materials.

Van der Waals epitaxy and characterization of hexagonal boron nitride nanosheets on graphene

Graphene is highly sensitive to environmental influences, and thus, it is worthwhile to deposit protective layers on graphene without impairing its excellent properties. Hexagonal boron nitride (h-BN), a well-known dielectric material, may afford the necessary protection. In this research, we demonstrated the van der Waals epitaxy of h-BN nanosheets on mechanically exfoliated graphene by chemical vapor deposition, using borazine as the precursor to h-BN. The h-BN nanosheets had a triangular morphology on a narrow graphene belt but a polygonal morphology on a larger graphene film. The h-BN nanosheets on graphene were highly crystalline, except for various in-plane lattice orientations. Interestingly, the h-BN nanosheets preferred to grow on graphene than on SiO2/Si under the chosen experimental conditions, and this selective growth spoke of potential promise for application to the preparation of graphene/h-BN superlattice structures fabricated on SiO2/Si.

Copper‐Vapor‐Assisted Rapid Synthesis of Large AB‐Stacked Bilayer Graphene Domains on Cu‐Ni Alloy

The synergic effects of Cu85Ni15 and the copper vapor evaporated from copper foil enabled the fast growth of a ≈300 μm bilayer graphene in ≈10 minutes. The copper vapor reduces the growth rate of the first graphene layer while the carbon dissolved in the alloy boosts the growth of the subsequently developed second graphene layer with an AB-stacking order.

Synthesis of High-Quality Graphene and Hexagonal Boron Nitride Monolayer In-Plane Heterostructure on Cu–Ni Alloy

Graphene/hexagonal boron nitride (h‐BN) monolayer in‐plane heterostructure offers a novel material platform for both fundamental research and device applications. To obtain such a heterostructure in high quality via controllable synthetic approaches is still challenging. In this work, in‐plane epitaxy of graphene/h‐BN heterostructure is demonstrated on Cu–Ni substrates. The introduction of nickel to copper substrate not only enhances the capability of decomposing polyaminoborane residues but also promotes graphene growth via isothermal segregation. On the alloy surface partially covered by h‐BN, graphene is found to nucleate at the corners of the as‐formed h‐BN grains, and the high growth rate for graphene minimizes the damage of graphene‐growth process on h‐BN lattice. As a result, high‐quality graphene/h‐BN in‐plane heterostructure with epitaxial relationship can be formed, which is supported by extensive characterizations. Photodetector device applications are demonstrated based on the in‐plane heterostructure. The success will have important impact on future research and applications based on this unique material platform.

Dielectric Breakdown in Chemical Vapor Deposited Hexagonal Boron Nitride

Insulating films are essential in multiple electronic devices because they can provide essential functionalities, such as capacitance effects and electrical fields. Two-dimensional (2D) layered materials have superb electronic, physical, chemical, thermal, and optical properties, and they can be effectively used to provide additional performances, such as flexibility and transparency. 2D layered insulators are called to be essential in future electronic devices, but their reliability, degradation kinetics, and dielectric breakdown (BD) process are still not understood. In this work, the dielectric breakdown process of multilayer hexagonal boron nitride (h-BN) is analyzed on the nanoscale and on the device level, and the experimental results are studied via theoretical models. It is found that under electrical stress, local charge accumulation and charge trapping/detrapping are the onset mechanisms for dielectric BD formation. By means of conductive atomic force microscopy, the BD event was triggered at several locations on the surface of different dielectrics (SiO2, HfO2, Al2O3, multilayer h-BN, and monolayer h-BN); BD-induced hillocks rapidly appeared on the surface of all of them when the BD was reached, except in monolayer h-BN. The high thermal conductivity of h-BN combined with the one-atom-thick nature are genuine factors contributing to heat dissipation at the BD spot, which avoids self-accelerated and thermally driven catastrophic BD. These results point to monolayer h-BN as a sublime dielectric in terms of reliability, which may have important implications in future digital electronic devices.