2D semiconductors can drive advances in quantum science and technologies. However, they should be free of any contamination; also, the crystallographic ordering and coupling of adjacent layers and their electronic properties should be well-controlled, tunable, and scalable. Here, these challenges are addressed by a new approach, which combines molecular beam epitaxy and in situ band engineering in ultra-high vacuum of semiconducting gallium selenide (GaSe) on graphene. In situ studies by electron diffraction, scanning probe microscopy, and angle-resolved photoelectron spectroscopy reveal that atomically-thin layers of GaSe align in the layer plane with the underlying lattice of graphene. The GaSe/graphene heterostructure, referred to as 2semgraphene, features a centrosymmetric (group symmetry D3d) polymorph of GaSe, a charge dipole at the GaSe/graphene interface, and a band structure tunable by the layer thickness. The newly-developed, scalable 2semgraphene is used in optical sensors that exploit the photoactive GaSe layer and the built-in potential at its interface with the graphene channel. This proof of concept has the potential for further advances and device architectures that exploit 2semgraphene as a functional building block.

Two-dimensional (2D) semiconductor field-effect film transistors combine large carrier mobility with mechanical flexibility and therefore can be ideally suitable for wearable electronics or at the sensor interfaces of smart sensor systems. However, such applications require large-area solution processing as opposed to single-flake devices, where the critical challenge to overcome is the high interflake resistance values. In this report, using a narrow-channel, near-vertical transport device architecture, we have fabricated inkjet-printed sub-20 nm channel electrolyte-gated transistors with predominantly intraflake carrier transport. Therefore, the electronics transport in these transistors is not dominated by the high interflake resistance, and the intraflake material properties including doping density, defect concentration, contact resistance, and threshold voltage modulation can be examined and optimized independently to achieve a current density as high as 280 μA·μm-1. In addition, through the passivation of the sulfur vacancies with a tailored surface treatment, we demonstrate an impressive On-Off current ratio exceeding 1 × 107, complemented by a low subthreshold swing of 100 mV·decade-1. Next, exploiting these high-performance transistors, unipolar depletion-load-type inverters have been fabricated that show a maximum gain of 31. Furthermore, we have realized NAND, NOR, and OR gates, demonstrating their seamless operation at a frequency of 1 kHz. Therefore, this work represents an important step forward to realize electronic circuits based on printed 2D thin film transistors.

Manipulation of excitonic emission in two-dimensional (2D) materials via the assembly of van der Waals (vdW) heterostructures unlocks numerous opportunities for engineering their photonic and optoelectronic properties. In this work, we introduce a category of mixed-dimensional vdW heterostructures, integrating 2D materials with one-dimensional (1D) semiconductor nanowires composed of vdW layers. This configuration induces spatially distinct localized excitonic emissions through a tailored interfacial heterolayer atomic arrangement. By precisely adjusting both the axial and sidewall facet orientations of bottom-up grown PbI2 vdW nanowires and by transferring them onto 1L WSe2 flakes, we establish vdW heterointerfaces with either perpendicular or parallel interatomic arrangements. The edge-standing heterojunction, featuring perpendicular PbI2 layers atop WSe2, promotes efficient charge transfer through the edges and coupled localized states, leading to an enhanced redshifted excitonic emission. Conversely, the layer-by-layer heterointerface, where PbI2 layers are in parallel contact with WSe2, exhibits substantial quenching due to deep midgap states in a type-II alignment, as evidenced by power-dependent measurements and first-principle calculations. Our results introduce a method for actively manipulating excitonic emissions in 2D transition metal dichalcogenides (TMDs) through edge engineering, highlighting their potential in the development of various quantum devices.

One of the exotic expectations in the 2D curved spacetime is the geometric potential from the curvature of the 2D space, still possessing unsolved fundamental questions through Dirac quantization. The atomically thin 2D materials are promising for the realization of the geometric potential, but the geometric potential in 2D materials is not identified experimentally. Here, the curvature-induced ring-patterned bound states are observed in structurally deformed 2D semiconductors and formulated the modified geometric potential for the curvature effect, which demonstrates the ring-shape bound states with angular momentum. The formulated modified geometric potential is analogous to the effective potential of a rotating charged black hole. Density functional theory and tight-binding calculations are performed, which quantitatively agree well with the results of the modified geometric potential. The modified geometric potential is described by modified Gaussian and mean curvatures, corresponding to the curvature-induced changes in spin-orbit interaction and band gap, respectively. Even for complex structural deformation, the geometric potential solves the complexity, which aligns well with experimental results. The understanding of the modified geometric potential provides us with an intuitive clue for quantum transport and a key factor for new quantum applications such as valleytronics, spintronics, and straintronics in 2D semiconductors.

A gate stack that facilitates a high-quality interface and tight electrostatic control is crucial for realizing high-performance and low-power field-effect transistors (FETs). However, when constructing conventional metal-oxide-semiconductor structures with two-dimensional (2D) transition metal dichalcogenide channels, achieving these requirements becomes challenging due to inherent difficulties in obtaining high-quality gate dielectrics through native oxidation or film deposition. Here, a gate-dielectric-less device architecture of van der Waals Schottky gated metal-semiconductor FETs (vdW-SG MESFETs) using a molybdenum disulfide (MoS2) channel and surface-oxidized metal gates such as nickel and copper is reported. Benefiting from the strong SG coupling, these MESFETs operate at remarkably low gate voltages, <0.5 V. Notably, they also exhibit Boltzmann-limited switching behavior featured by a subthreshold swing of ≈60 mV dec-1 and negligible hysteresis. These ideal FET characteristics are attributed to the formation of a Fermi-level (EF) pinning-free gate stack at the Schottky-Mott limit. Furthermore, authors experimentally and theoretically confirm that EF depinning can be achieved by suppressing both metal-induced and disorder-induced gap states at the interface between the monolithic-oxide-gapped metal gate and the MoS2 channel. This work paves a new route for designing high-performance and energy-efficient 2D electronics.

2D semiconductors have interesting physical and chemical attributes that have led them to become one of the most intensely investigated semiconductor families in recent history. They may play a crucial role in the next technological revolution in electronics as well as optoelectronics or photonics. In this Perspective, we explore the fundamental principles and significant advancements in electronic and photonic devices comprising 2D semiconductors. We focus on strategies aimed at enhancing the performance of conventional devices and exploiting important properties of 2D semiconductors that allow fundamentally interesting device functionalities for future applications. Approaches for the realization of emerging logic transistors and memory devices as well as photovoltaics, photodetectors, electro-optical modulators, and nonlinear optics based on 2D semiconductors are discussed. We also provide a forward-looking perspective on critical remaining challenges and opportunities for basic science and technology level applications of 2D semiconductors.

The electronic properties of 2D materials are highly influenced by the molecular activity at their interfaces. A method was proposed to address this issue by employing passivation techniques using monolayer MoS2 field-effect transistors (FETs) while preserving high performance. Herein, we have used alkali metal fluorides as dielectric capping layers, including lithium fluoride (LiF), sodium fluoride (NaF), and potassium fluoride (KF) dielectric capping layers, to mitigate the environmental impact of oxygen and water exposure. Among them, the LiF dielectric capping layer significantly improved the transistor performance, specifically in terms of enhanced field effect mobility from 74 to 137 cm2/V·s, increased current density from 17 μA/μm to 32.13 μA/μm at a drain voltage of Vd of 1 V, and decreased subthreshold swing to 0.8 V/dec The results have been analytically verified by X-ray photoelectron spectroscopy (XPS) and Raman, and photoluminescence (PL) spectroscopy, and the demonstrated technique can be extended to other transition metal dichalcogenide (TMD)-based FETs, which can become a prospect for cutting-edge electronic applications. These findings highlight certain important trade-offs and provide insight into the significance of interface control and passivation material choice on the electrical stability, performance, and enhancement of the MoS2 FET.

Monolayer 2D semiconductors, such as WS2, exhibit uniquely strong light-matter interactions due to exciton resonances that enable atomically thin optical elements. Similar to geometry-dependent plasmon and Mie resonances, these intrinsic material resonances offer coherent and tunable light scattering. Thus far, the impact of the excitons\' temporal dynamics on the performance of such excitonic metasurfaces remains unexplored. Here, we show how the excitonic decay rates dictate the focusing efficiency of an atomically thin lens carved directly out of exfoliated monolayer WS2. By isolating the coherent exciton radiation from the incoherent background in the focus of the lens, we obtain a direct measure of the role of exciton radiation in wavefront shaping. Furthermore, we investigate the influence of exciton-phonon scattering by characterizing the focusing efficiency as a function of temperature, demonstrating an increased optical efficiency at cryogenic temperatures. Our results provide valuable insights into the role of excitonic light scattering in 2D nanophotonic devices.

Curvature is a general factor for various two-dimensional (2D) materials due to their flexibility, which is not yet fully unveiled to control their physical properties. In particular, the effect of structural disorder with random curvature formation on excitons in 2D semiconductors is not fully understood. Here, the correlation between structural disorder and exciton formation in monolayer MoS2 on SiO2 was investigated by using photoluminescence (PL) and Raman spectroscopy. We found that the curvature-induced charge localization along with band gap fluctuations aid the formation of the localized charged excitons (such as trions). In the substrate-supported region, the trion population is enhanced by a localized charge due to the microscopic random bending strain, while the trion is suppressed in the suspended region which exhibits negligible bending strain, anomalously even though the dielectric screening effect is lower than that of the supported region. The redistribution of each exciton by the bending strain leads to a huge variation (∼100-fold) in PL intensity between the supported and suspended regions, which cannot be fully comprehended by external potential disorders such as a random distribution of charged impurities. The peak position of PL in MoS2/SiO2 is inversely proportional to the Raman peak position of E12g, indicating that the bending strain is correlated with PL. The supported regions exhibit an indirect portion that was not shown in the suspended regions or atomically flat substrates. The understanding of the structural disorder effect on excitons provides a fundamental path for optoelectronics and strain engineering of 2D semiconductors.

Two-dimensional (2D) semiconductors have recently attracted considerable attention due to their promising applications in future integrated electronic and optoelectronic devices. Large-scale synthesis of high-quality 2D semiconductors is an increasingly essential requirement for practical applications, such as sensing, imaging, and communications. In this work, homogeneous 2D GaTe films on a centimeter scale are epitaxially grown on fluorphlogopite mica substrates by molecular beam epitaxy (MBE). The epitaxial GaTe thin films showed an atomically 2D layered lattice structure with a T phase, which has not been discovered in the GaTe geometric isomer. Furthermore, semiconducting behavior and high mobility above room temperature were found in T-GaTe epitaxial films, which are essential for application in semiconducting devices. The T-GaTe-based photodetectors demonstrated respectable photodetection performance with a responsivity of 13 mA/W and a fast response speed. By introducing monolayer graphene as the substrate, we successfully realized high-quality GaTe/graphene heterostructures. The performance has been significantly improved, such as the responsivity was enhanced more than 20 times. These results highlight a feasible scheme for exploring the crystal phase of 2D GaTe and realizing the controlled growth of GaTe films on large substrates, which could promote the development of broadband, high-performance, and large-scale photodetection applications.