We establish a powerful poly(4-styrenesulfonate) (PSS)-treated strategy for sulfur vacancy healing in monolayer MoS2 to precisely and steadily tune its electronic state. The self-healing mechanism, in which the sulfur vacancies are healed spontaneously by the sulfur adatom clusters on the MoS2 surface through a PSS-induced hydrogenation process, is proposed and demonstrated systematically. The electron concentration of the self-healed MoS2 dramatically decreased by 643 times, leading to a work function enhancement of ∼150 meV. This strategy is employed to fabricate a high performance lateral monolayer MoS2 homojunction which presents a perfect rectifying behaviour, excellent photoresponsivity of ∼308 mA W−1 and outstanding air-stability after two months. Unlike previous chemical doping, the lattice defect-induced local fields are eliminated during the process of the sulfur vacancy self-healing to largely improve the homojunction performance. Our findings demonstrate a promising and facile strategy in 2D material electronic state modulation for the development of next-generation electronics and optoelectronics.

The applications of any two-dimensional (2D) semiconductor devices cannot bypass the control of metal-semiconductor interfaces, which can be severely affected by complex Fermi pinning effects and defect states. Here, we report a near-ideal rectifier in the all-2D Schottky junctions composed of the 2D metal 1 T′-MoTe2 and the semiconducting monolayer MoS2. We show that the van der Waals integration of the two 2D materials can efficiently address the severe Fermi pinning effect generated by conventional metals, leading to increased Schottky barrier height. Furthermore, by healing original atom-vacancies and reducing the intrinsic defect doping in MoS2, the Schottky barrier width can be effectively enlarged by 59%. The 1 T′-MoTe2/healed-MoS2 rectifier exhibits a near-unity ideality factor of ~1.6, a rectifying ratio of >5 × 105, and high external quantum efficiency exceeding 20%. Finally, we generalize the barrier optimization strategy to other Schottky junctions, defining an alternative solution to enhance the performance of 2D-material-based electronic devices.

Monolayer 2D semiconductors (e.g., MoS2) are of considerable interest for atomically thin transistors but generally limited by insufficient carrier mobility or driving current. Minimizing the lattice defects in 2D semiconductors represents a common strategy to improve their electronic properties, but has met with limited success to date. Herein, a hidden benefit of the atomic vacancies in monolayer 2D semiconductors to push their performance limit is reported. By purposely tailoring the sulfur vacancies (SVs) to an optimum density of 4.7% in monolayer MoS2, an unusual mobility enhancement is obtained and a record‐high carrier mobility (>115 cm2 V−1 s−1) is achieved, realizing monolayer MoS2 transistors with an exceptional current density (>0.60 mA µm−1) and a record‐high on/off ratio >1010, and enabling a logic inverter with an ultrahigh voltage gain >100. The systematic transport studies reveal that the counterintuitive vacancy‐enhanced transport originates from a nearest‐neighbor hopping conduction model, in which an optimum SV density is essential for maximizing the charge hopping probability. Lastly, the vacancy benefit into other monolayer 2D semiconductors is further generalized; thus, a general strategy for tailoring the charge transport properties of monolayer materials is defined.

van der Waals (vdWs) heterostructures have provided a platform for nanoscale material integrations and enabled promise for use in optoelectronic devices. Because of the ultrastrength of two-dimensional materials, strain engineering is considered as an effective way to tune their band structures and further tailor the interface performance of vdWs heterostructures. However, the less-constrained vdWs interfaces make the traditional strain technique via latticemismatched growth infeasible. Here, we report a strategy to construct mixed-dimensional heterostructure arrays with periodically strain-engineered vdWs interfaces utilizing one-dimensional semiconductor-induced nanoindentation. Using monolayer MoS 2 (1L-MoS 2 )/ZnO heterostructure arrays as a model system, we demonstrate inhomogeneous built-in strain gradient at the heterointerfaces ranging from 0 to 0.6% tensile. Through systematic optical characterization of the hybrid structures, we verify that strain can improve the interfacial charge transfer efficiency. Consequently, we observe that the photoluminescence (PL) emission of 1L-MoS 2 at strained interfaces is dramatically quenched more than 50% with respect to that at unstrained interfaces. Furthermore, we confirm that the strain-optimized interfacial carrier behavior is attributed to the reduction of interfacial barrier height, which originated from the strain-dependent Fermi level of 1L-MoS 2 . These results demonstrate that strain provides another degree of freedom in tuning the vdWs interface performance and our method developed here should enable flexibility in achieving more sophisticated vdWs integration via strain engineering.

Ultrathin molybdenum disulfide (MoS2) presents ideal properties for building next‐generation atomically thin circuitry. However, it is difficult to construct logic units of MoS2 monolayer using traditional silicon‐based doping schemes, such as atomic substitution and ion implantation, as they cause lattice disruption and doping instability. An accurate and feasible electronic structure modulation strategy from defect engineering is proposed to construct homogeneous electronics for MoS2 monolayer logic inverters. By utilizing the energy‐matched electron induction of the solution process, numerous pure and lattice‐stable monosulfur vacancies (Vmonos) are introduced to modulate the electronic structure of monolayer MoS2 via a shallow trapping effect. The resulting modulation effectively reduces the electronic concentration of MoS2 and improves the work function by 100 meV. Under modulation of Vmonos, an atomically thin homogenous monolayer MoS2 logic inverter with a voltage gain of 4 is successfully constructed. A brand‐new and practical design route of defect modulation for 2D‐based circuit development is provided.