Seamless stitching of graphene domains on polished copper (111) is proved clearly not only at atomic scale by scanning tunnelling microscopy (STM) and transmission electron micoscopy (TEM), but also at the macroscale by optical microscopy after UV-treatment. Using this concept of seamless stitching, synthesis of 6 cm × 3 cm monocrystalline graphene without grain boundaries on polished copper (111) foil is possible, which is only limited by the chamber size.

Graphene has attracted significant interest both for exploring fundamental science and for a wide range of technological applications. Chemical vapor deposition (CVD) is currently the only working approach to grow graphene at wafer scale, which is required for industrial applications. Unfortunately, CVD graphene is intrinsically polycrystalline, with pristine graphene grains stitched together by disordered grain boundaries, which can be either a blessing or a curse. On the one hand, grain boundaries are expected to degrade the electrical and mechanical properties of polycrystalline graphene, rendering the material undesirable for many applications. On the other hand, they exhibit an increased chemical reactivity, suggesting their potential application to sensing or as templates for synthesis of one-dimensional materials. Therefore, it is important to gain a deeper understanding of the structure and properties of graphene grain boundaries. Here, we review experimental progress on identification and electrical and chemical characterization of graphene grain boundaries. We use numerical simulations and transport measurements to demonstrate that electrical properties and chemical modification of graphene grain boundaries are strongly correlated. This not only provides guidelines for the improvement of graphene devices, but also opens a new research area of engineering graphene grain boundaries for highly sensitive electro-biochemical devices.

Semiconducting transition metal dichalcogenides (TMDs) are promising materials for photodetection over a wide range of visible wavelengths. Photodetection is generally realized via a phototransistor, photoconductor, p-n junction photovoltaic device, and thermoelectric device. The photodetectivity, which is a primary parameter in photodetector design, is often limited by either low photoresponsivity or a high dark current in TMDs materials. Here, we demonstrated a highly sensitive photodetector with a MoS/h-BN/graphene heterostructure, by inserting a h-BN insulating layer between graphene electrode and MoS photoabsorber, the dark-carriers were highly suppressed by the large electron barrier (2.7 eV) at the graphene/h-BN junction while the photocarriers were effectively tunneled through small hole barrier (1.2 eV) at the MoS/h-BN junction. With both high photocurrent/dark current ratio (>10) and high photoresponsivity (180 AW), ultrahigh photodetectivity of 2.6 × 10 Jones was obtained at 7 nm thick h-BN, about 100-1000 times higher than that of previously reported MoS-based devices.

Concepts of non-volatile memory to replace conventional flash memory have suffered from low material reliability and high off-state current, and the use of a thick, rigid blocking oxide layer in flash memory further restricts vertical scale-up. Here, we report a two-terminal floating gate memory, tunnelling random access memory fabricated by a monolayer MoS2/h-BN/monolayer graphene vertical stack. Our device uses a two-terminal electrode for current flow in the MoS2 channel and simultaneously for charging and discharging the graphene floating gate through the h-BN tunnelling barrier. By effective charge tunnelling through crystalline h-BN layer and storing charges in graphene layer, our memory device demonstrates an ultimately low off-state current of 10−14 A, leading to ultrahigh on/off ratio over 109, about ∼103 times higher than other two-terminal memories. Furthermore, the absence of thick, rigid blocking oxides enables high stretchability (>19%) which is useful for soft electronics.

Memristors such as phase-change memory and resistive memory have been proposed to emulate the synaptic activities in neuromorphic systems. However, the low reliability of these types of memories is their biggest challenge for commercialization. Here, a highly reliable memristor array using floating-gate memory operated by two terminals (source and drain) using van der Waals layered materials is demonstrated. Centimeter-scale samples (1.5 cm × 1.5 cm) of MoS as a channel and graphene as a trap layer grown by chemical vapor deposition (CVD) are used for array fabrication with Al O as the tunneling barrier. With regard to the memory characteristics, 93% of the devices exhibit an on/off ratio of over 10 with an average ratio of 10 . The high on/off ratio and reliable endurance in the devices allow stable 6-level memory applications. The devices also exhibit excellent memory durability over 8000 cycles with a negligible shift in the threshold voltage and on-current, which is a significant improvement over other types of memristors. In addition, the devices can be strained up to 1% by fabricating on a flexible substrate. This demonstration opens a practical route for next-generation electronics with CVD-grown van der Waals layered materials.

Aside from unusual properties of monolayer graphene, bilayer has been shown to have even more interesting physics, in particular allowing bandgap opening with dual gating for proper interlayer symmetry. Such properties, promising for device applications, ignited significant interest in understanding and controlling the growth of bilayer graphene. Here we systematically investigate a broad set of flow rates and relative gas ratio of CH to H in atmospheric pressure chemical vapor deposition of multilayered graphene. Two very different growth windows are identified. For relatively high CH to H ratios, graphene growth is relatively rapid with an initial first full layer forming in seconds upon which new graphene flakes nucleate then grow on top of the first layer. The stacking of these flakes versus the initial graphene layer is mostly turbostratic. This growth mode can be likened to Stranski-Krastanov growth. With relatively low CH to H ratios, growth rates are reduced due to a lower carbon supply rate. In addition bi-, tri-, and few-layer flakes form directly over the Cu substrate as individual islands. Etching studies show that in this growth mode subsequent layers form beneath the first layer presumably through carbon radical intercalation. This growth mode is similar to that found with Volmer-Weber growth and was shown to produce highly oriented AB-stacked materials. These systematic studies provide new insight into bilayer graphene formation and define the synthetic range where gapped bilayer graphene can be reliably produced.

Single-crystalline artificial AB-stacked bilayer graphene is formed by aligned transfer of two single-crystalline monolayers on a wafer-scale. The obtained bilayer has a well-defined interface and is electronically equivalent to exfoliated or direct-grown AB-stacked bilayers.

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