Stack growth of wafer-scale van der Waals superconductor heterostructures.

Two-dimensional (2D) van der Waals (vdW) heterostructures have attracted considerable attention in recent years1-5. The most widely used method of fabrication is to stack mechanically exfoliated micrometre-sized flakes6-18, but this process is not scalable for practical applications. Despite thousands of 2D materials being created, using various stacking combinations1-3,19-21, hardly any large 2D superconductors can be stacked intact into vdW heterostructures, greatly restricting the applications for such devices. Here we report a high-to-low temperature strategy for controllably growing stacks of multiple-layered vdW superconductor heterostructure (vdWSH) films at a wafer scale. The number of layers of 2D superconductors in the vdWSHs can be precisely controlled, and we have successfully grown 27 double-block, 15 triple-block, 5 four-block and 3 five-block vdWSH films (where one block represents one 2D material). Morphological, spectroscopic and atomic-scale structural analyses reveal the presence of parallel, clean and atomically sharp vdW interfaces on a large scale, with very little contamination between neighbouring layers. The intact vdW interfaces allow us to achieve proximity-induced superconductivity and superconducting Josephson junctions on a centimetre scale. Our process for making multiple-layered vdWSHs can easily be generalized to other situations involving 2D materials, potentially accelerating the design of next-generation functional devices and applications22-24.

Controllable growth of wafer-scale monolayer transition metal dichalcogenides ternary alloys with tunable band gap.

The tuning of band gap is very important for the application of two-dimensional (2D) materials in optoelectronic devices. Alloying of 2D transition metal dichalcogenides (TMDCs) is an important way to tune the wide band gap. In this study, we report a multi-step vapor deposition method to grow monolayer TMDC ternary alloy films with wafer scale, including Mo1-xWxS2, Mo1-xWxSe2and MoS2xSe2(1-x), which are accurately controllable in the elemental proportion (xis from 0 to 1). The band gap of the three 2D ternary alloy materials are continuously tuned for the whole range of metal and chalcogen compositions. The metal compositions are controlled by the as-deposited thickness. Raman, photoluminescence, elemental maps and TEM show the high spatial homogeneity in the compositions and optical properties across the whole wafer. The band gap can be continuously tuned from 1.86 to 1.99 eV for Mo1-xWxS2, 1.56 to 1.65 eV for Mo1-xWxSe2, 1.56 to 1.86 eV for MoS2xSe2(1-x). Electrical transport measurements indicate that Mo1-xWxS2and MoS2xSe2(1-x)monolayers shown-type semiconductor behaviors, and the carrier types of Mo1-xWxSe2can be tuned asn-type, bipolar andp-type. Moreover, this control process can be easily generalized to other 2D alloy films, even to quaternary or multi-element alloy materials. Our study presents a promising route for the preparation of large-scale homogeneous monolayer TMDC alloys and the application for future functional devices.

Controllable defects in monolayer graphene induced by hydrogen and argon plasma.

Graphene has attracted wide attentions since its successfully exfoliation. Honeycombsp2carbon lattice and Dirac semi-metal band structure make graphene a promising material with excellent mechanical strength, thermal conductivity, and carrier mobility. However, the absence of intrinsic bandgap limits its application in semiconductor. Defects in graphene is supposed to modify its band structure and lead to an opened bandgap. Many methods have been demonstrated to introduce defects into graphene, such as chemical reaction, plasma, electron beam, and laser. However, the species of defects are mostly uncontrollable in most treatment processes. In this study, we report three kinds of defects can be controllably induced in graphene via hydrogen (H2) and argon (Ar) plasma. With different parameter and feeding gas, hydrogenated graphene, graphene nanomesh and graphene with vacancies can be well obtained. The defect density can be precisely controlled by tuning plasma power and irradiation time. Morphological, spectroscopic, and electrical characterizations are performed to systematically investigate the defect evolution. Graphene nanomesh and graphene with vacancies show obvious difference for roughness and coverage, whereas the morphology of hydrogenated graphene remains similar with that of as-prepared graphene. For hydrogenated graphene, an opened bandgap of ∼20 meV is detected. For graphene nanomesh and graphene with vacancies, the semiconductive on/off behaviors are observed. We believe this work can provide more details of plasma-induced defects and assist the application of graphene in semiconductor industry.

Stacking transfer of wafer-scale graphene-based van der Waals superlattices.

High-quality graphene-based van der Waals superlattices are crucial for investigating physical properties and developing functional devices. However, achieving homogeneous wafer-scale graphene-based superlattices with controlled twist angles is challenging. Here, we present a flat-to-flat transfer method for fabricating wafer-scale graphene and graphene-based superlattices. The aqueous solution between graphene and substrate is removed by a two-step spinning-assisted dehydration procedure with the optimal wetting angle. Proton-assisted treatment is further used to clean graphene surfaces and interfaces, which also decouples graphene and neutralizes the doping levels. Twist angles between different layers are accurately controlled by adjusting the macroscopic stacking angle through their wafer flats. Transferred films exhibit minimal defects, homogeneous morphology, and uniform electrical properties over wafer scale. Even at room temperature, robust quantum Hall effects are observed in graphene films with centimetre-scale linewidth. Our stacking transfer method can facilitate the fabrication of graphene-based van der Waals superlattices and accelerate functional device applications.

Tuning the morphology of 2D transition metal chalcogenides via oxidizing conditions.

Two-dimensional transition metal chalcogenides (TMCs) are emerging as an intriguing platform to realize nascent properties in condensed matter physics, materials science and device engineering. Controllable growing of TMCs becomes increasingly important, especially for the layer number, doping, and morphology. Here, we successfully tune the morphology of MoS2, MoSe2, WS2and WSe2, from homogenous films to individual single crystalline grains only via changing the oxidizing growth conditions. The oxidization degrees are determined by the oxygen that adsorbed on substrates and the oxygen concentrations in reaction gas together. We find the homogenous films are easily formed under the reductive conditions, triangular grains prefer the weak oxidizing conditions, and medium oxidizing conditions bring in dendritic grains with higher oxygen doping and inhomogenous photoluminescence intensities from edge to interior regions shown in the dendritic grains. These growth rules under different oxidizing conditions are easily generalized to other TMCs, which also show potential for growing specific TMCs with designed oxygen doping levels.