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Various 2D materials can be assembled into vertical heterostructure stacks that emit strong electroluminescence. However, to date, most work is done using mechanical exfoliated materials, with little insights gained into the operation limits and failure mechanisms due to the limited number of devices produced and the device-to-device variances. However, when using chemical vapor deposition (CVD) grown 2D crystals, it is possible to construct dozens of devices to generate statistics and ensemble insights, providing a viable way toward scalable industrialization of 2D optoelectronics. In particular, the operation lifetime/duration of electroluminescence and subsequent failure mechanisms are poorly understood. Here, we demonstrate that all-2D vertical layered heterostructure (VLH) devices made using CVD-grown materials (Gr:h-BN:WS 2 :h-BN:Gr) can generate strong red electroluminescence (EL) with continuous operation for more than 2 h in ambient atmospheric conditions under constant bias. Layer-by-layer controlled assembly is used to achieve graphene top and bottom electrodes in a crossbar geometry, with few layered h-BN continuous films as tunnel barriers for direct carrier injection into semiconducting monolayer WS 2 single crystals with direct band gap recombination. Tens of the devices were fabricated in a single chip, with strong EL routinely measured under both positive and negative graphene electrode bias. The success rate for EL emission in devices is over 90%. EL starts to be detected at bias values of ∼5 V, with bright red emission located at the crossbar intersection site, with intensity increasing with applied bias. Long-lived persistent EL is demonstrated for more than 2 h without significant degradation of WS 2 under high bias conditions of 20 V. In cycling tests, the EL signal peak position and intensity stay almost the same after several ON/OFF cycles with high bias, which proves that our device has good stability and durability when pulsed. Breakdown of the device is shown to occur at a bias value of ∼35 V, whereby current reduces to zero and EL abruptly stops, due to breakdown of the top graphene electrode, associated with local heating accumulation. This study provides a viable way for wafer-scale fabrication of high-performance 2D EL arrays for ultrathin optoelectronic devices and sheds light on the mechanisms of failure and operation limits of EL devices in ambient conditions.

Heterophase homojunction formation in atomically thin 2D layers is of great importance for next-generation nanoelectronics and optoelectronics applications. Technologically challenging, controllable transformation between the semiconducting and metallic phases of transition metal chalcogenides is of particular importance. Here, we demonstrate that controlled laser irradiation can be used to directly ablate PdSe 2 thin films using high power or trigger the local transformation of PdSe 2 into a metallic phase PdSe 2- x using lower laser power. Such transformations are possible due to the low decomposition temperature of PdSe 2 and a variety of stable phases compared to other 2D transition metal dichalcogenides. Scanning transmission electron microscopy is used to reveal the laser-induced Se-deficient phases of PdSe 2 material. The process sensitivity to the laser power allows patterning flexibility for resist-free device fabrication. The laser-patterned devices demonstrate that a laser-induced metallic phase PdSe 2- x is stable with increased conductivity by a factor of about 20 compared to PdSe 2 . These findings contribute to the development of nanoscale devices with homojunctions and scalable methods to achieve structural transformations in 2D materials.