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Developing future electronics will require aggressive scaling of the channel material thickness while maintaining device performance. Two-dimensional (2D) semiconductors are promising candidates to sustain further device scaling, but despite more than two decades of intense research, experimental performance continues to lag theoretical expectations. Here, we develop an oxygen-free approach to fabricate 2D field-effect transistors and push the electrical transport toward the theoretical phonon-limited intrinsic mobility. This approach achieves record carrier mobilities of 91 and 132 cm 2 V -1 s -1 for mono- and bilayer MoS 2 transistors on silicon oxide substrates. Statistical analysis of over 60 MoS 2 and WS 2 devices confirms that oxygen-free fabrication enhances device performance by more than an order of magnitude across key figures of merit. While previous studies suggest that 2D transition metal dichalcogenides such as MoS 2 and WS 2 are relatively stable in air, we show that even short-term ambient exposure can degrade their performance. We identify oxygen as a crucial factor in limiting transistor performance through irreversible chemisorption. This study emphasizes the criticality of avoiding oxygen exposure and offers guidance for device manufacturing that impacts fundamental research and practical applications of 2D materials.

Two-dimensional van der Waals semiconductors are promising for future nanoelectronics. However, integrating high-k gate dielectrics for device applications is challenging as the inert van der Waals material surfaces hinder uniform dielectric growth. Here, we report a liquid metal oxide-assisted approach to integrate ultrathin, high-k HfO 2 dielectric on 2D semiconductors with atomically smooth interfaces. Using this approach, we fabricated 2D WS 2 top-gated transistors with subthreshold swings down to 74.5 mV/dec, gate leakage current density below 10 -6 A/cm 2 , and negligible hysteresis. We further demonstrate a one-step van der Waals integration of contacts and dielectrics on graphene. This can offer a scalable approach toward integrating entire prefabricated device stack arrays with 2D materials. Our work provides a scalable solution to address the crucial dielectric engineering challenge for 2D semiconductor-based electronics.

Semiconducting transition metal dichalcogenides (TMDs) are a class of two-dimensional materials with potential applications in optoelectronics, spintronics, valleytronics, and quantum information processing. Understanding their stability under ambient conditions is critical for determining their in-air processability during device fabrication and for predicting their long-term device performance stability. While the effects of environmental conditions (i.e., oxygen, moisture, and light) on TMD degradation are well-acknowledged, the role of defects in driving their oxidation remains unclear. We conducted a systematic X-ray photoelectron spectroscopy study on WS 2 single crystals with different surface S-vacancy concentrations formed via controlled argon sputtering. Oxidation primarily occurred at defect concentrations ≥ 10%, resulting in stoichiometric WO 3 formation, while a stable surface was observed at lower concentrations. Theoretical calculations informed us that single S-vacancies do not spontaneously oxidize, while defect pairing at high vacancy concentrations facilitates O 2 dissociation and subsequent oxide formation. Our XPS results also point to vacancy-related structural and electrostatic disorder as the main origin for the p-type characteristics that persists even after oxidation. Despite the complex interplay between defects and TMD oxidation processes, our work unveils scientifically informed guidance for working effectively with TMDs.

The manipulation of edge configurations and structures in atomically-thin transition metal dichalcogenides (TMDs) for versatile functionalization has attracted intensive interest in recent years. The chemical vapor deposition (CVD) approach has shown promise for TMD edge engineering of atomic edge configurations (1H, 1T or 1T'-zigzag or armchair edges) as well as diverse edge morphologies (1D nanoribbons, 2D dendrites, 3D spirals, etc.). These edge-rich TMD layers offer versatile candidates for probing the physical and chemical properties and exploring potential applications in electronics, optoelectronics, catalysis, sensing, and quantum technologies. In this Review, we present an overview of the current state-of-the-art in the manipulation of TMD atomic edges and edge-rich structures using CVD. We highlight the vast range of distinct properties associated with these edge configurations and structures and provide insights into the opportunities afforded by such edge-functionalized crystals. The objective of this Review is to motivate further research and development efforts to use CVD as a scalable approach to harness the benefits of such crystal-edge engineering.

Two-dimensional (2D) semiconductors are promising channel materials for continued downscaling of complementary metal-oxide-semiconductor (CMOS) logic circuits. However, their full potential continues to be limited by a lack of scalable high- k dielectrics that can achieve atomically smooth interfaces, small equivalent oxide thicknesses (EOTs), excellent gate control, and low leakage currents. Here, large-area liquid-metal-printed ultrathin Ga 2 O 3 dielectrics for 2D electronics and optoelectronics are reported. The atomically smooth Ga 2 O 3 /WS 2 interfaces enabled by the conformal nature of liquid metal printing are directly visualized. Atomic layer deposition compatibility with high- k Ga 2 O 3 /HfO 2 top-gate dielectric stacks on a chemical-vapor-deposition-grown monolayer WS 2 is demonstrated, achieving EOTs of ∼1 nm and subthreshold swings down to 84.9 mV/dec. Gate leakage currents are well within requirements for ultrascaled low-power logic circuits. These results show that liquid-metal-printed oxides can bridge a crucial gap in dielectric integration of 2D materials for next-generation nanoelectronics.

Making electrical contacts to semiconducting transition metal dichalcogenides (TMDCs) represents a major bottleneck for high device performance, often manifesting as strong Fermi level pinning and high contact resistance. Despite intense ongoing research, the mechanism by which lattice defects in TMDCs impact the transport properties across the contact-TMDC interface remains unsettled. Here we study the impact of S-vacancies on the electronic properties at a MoS 2 monolayer interfaced with graphite by photoemission spectroscopy, where the defect density is selectively controlled by Ar sputtering. A clear reduction of the MoS 2 core level and valence band binding energies is observed as the defect density increases. The experimental results are explained in terms of (i) gap states' energy distribution and (ii) S-vacancies' electrostatic disorder effect. Our model indicates that the Fermi level pinning at deep S-vacancy gap states is the origin of the commonly reported large electron injection barrier (∼0.5 eV) at the MoS 2 ML interface with low work function metals. At the contact with high work function electrodes, S-vacancies do not significantly affect the hole injection barrier, which is intrinsically favored by Fermi level pinning at shallow occupied gap states. Our results clarify the importance of S-vacancies and electrostatic disorder in TMDC-based electronic devices, which could lead to strategies for optimizing device performance and production.

We present a combined experimental and theoretical study of monolayer vanadium ditelluride, VTe 2 , grown on highly oriented pyrolytic graphite by molecular-beam epitaxy. Using various in situ microscopic and spectroscopic techniques, including scanning tunneling microscopy/spectroscopy, synchrotron X-ray and angle-resolved photoemission, and X-ray absorption, together with theoretical analysis by density functional theory calculations, we demonstrate direct evidence of the metallic 1T phase and 3d 1 electronic configuration in monolayer VTe 2 that also features a (4 × 4) charge density wave order at low temperatures. In contrast to previous theoretical predictions, our element-specific characterization by X-ray magnetic circular dichroism rules out a ferromagnetic order intrinsic to the monolayer. Our findings provide essential knowledge necessary for understanding this interesting yet less explored metallic monolayer in the emerging family of van der Waals magnets.

Single-layer molybdenum disulfide (MoS 2 ) has attracted significant attention due to its electronic and physical properties, with much effort invested toward obtaining large-area high-quality monolayer MoS 2 films. In this work, we demonstrate a reactive-barrier-based approach to achieve growth of highly homogeneous single-layer MoS 2 on sapphire by the use of a nickel oxide foam barrier during chemical vapor deposition. Due to the reactivity of the NiO barrier with MoO 3 , the concentration of precursors reaching the substrate and thus nucleation density is effectively reduced, allowing grain sizes of up to 170 μm and continuous monolayers on the centimeter length scale being obtained. The quality of the monolayer is further revealed by angle-resolved photoemission spectroscopy measurement by observation of a very well resolved electronic band structure and spin-orbit splitting of the bands at room temperature with only two major domain orientations, indicating the successful growth of a highly crystalline and well-oriented MoS 2 monolayer.