Operational Limits and Failure Mechanisms in All-2D van der Waals Vertical Heterostructure Devices with Long-Lived...

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:WS₂: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 WS₂ 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 WS₂ 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.